A theoretical study on electron transfer in low-energy collisions of a collinear meta-stable with a $ {\rm{Na}}_3^ - $ {\rm{Na}}_3^ - " border="0"> Na

Electron transfer in the collisions of a with a Na is theoretically studied. It is assumed that the target is collinear (D _h ) and that its electronic state is meta-stable triplet state. Adiabatic potential energy surfaces and non-adiabatic couplings of the system are calculated by using a semi-empirical diatomics-in-molecules (DIM) method. The positions of (avoided)-crossings of potential surfaces are investigated and the non-adiabatic couplings between two different electronic states are calculated. An avoided crossing is found in the region where the separation between the target and projectile is relatively large (10–15 bohr). A dynamical calculation demonstrates that this crossing causes charge transfer between the target and projectile. Another intersection at a smaller separation changes the targets spin state (from triplet state to singlet state or vice versa). The cross-sections for charge and spin transfer reaction are estimated at the collision energy of 6.8 keV. It is found that the charge transfer cross-section is extremely enhanced when the target cluster ion is in its meta-stable triplet state comared to the case where the cluster is the ground singlet state.     

Charge transfer between alkali cluster ions and atoms in the 1 to 10 keV collisional energy range

The cross-sections for collisional charge transfer between singly charged free clusters M _n ⁺ (M = Li, Na; n=1...50) and atomic targets A (cesium, potassium) have been measured as a function of collisional relative velocity in laboratory energy range 1–10 keV. For each cluster size, the experimental values of the charge transfer cross-section are fitted with an universal parametric curve with two independent parameters and v_m, the maximum cross-section and the corresponding velocity. For small size clusters (), the characteristic parameters show strong variations with the number of atoms in the cluster. Abrupt dips observed for n=10 and n=22 are attributed to electronic properties. Charge transfer patterns observed for various collisional systems present similarities, which appear more sensitive to cluster quantum size effects than to collision energy defects. In their whole, the and v_m parameters show differences in both their size evolution and their absolute values discussed in term of projectile and target electronic structures. Received 13 April 2000 and Received in final form 29 June 2000     

Electron detachment and fragmentation in collisions between 1.25 keV/carbon and clusters and

The destruction cross-section for 22.5 and 50 keV C^1- , for 10 and 50 keV C₈ ^1- and for 50 and 75 keV C₆₀ ^1- clusters in collisions with H₂ has been measured by an attenuation method. The destruction of the cluster anions is dominated by electron detachment rather than fragmentation and is of the order of the geometric cross-section. The cross-sections vary little with bombarding energy. Received: 16 September 1998 / Received in final form: 23 February 1999     

The influence of O and C doping on the ionization potentials of Li-clusters

The influence of doping of Li-clusters by electronegative O and C atoms on the ionization potentials was investigated. Experimentally, we report ionization potentials for bare Li_n clusters deduced from photoionization efficiency spectra. The values are compared with the results for Li_nO and Li_nC clusters. Observed differences are largely attributed to a quantum size effect caused by the segregated molecular part around the impurity, which changes the electron work function. Theoretically, the Fermi and exchange-correlation energies which enter the work function, are calculated in the frame of the augmented plane wave (APW) method by taking explicitly into account the presence of the molecular core. The other contribution to the work function, the moment of the double layer at the cluster surface, is computed by solving the corresponding Poisson's equation. Received 9 September 1999 and Received in final form 7 February 2000     

Electronic correlation effects on the properties of an half-filled octahedron cluster in a magnetic field

The present study focuses on electronic correlation effects on magnetic energy, the spin-spin correlation function of an octahedron cluster in the (3↑, 3 ↓) electronic configuration threaded by a magnetic field. Some other spin configurations are also discussed and various field directions are considered. An accurate diagonalisation technique has been used to solve the Hubbard Hamiltonian. A result is analysed on a linear energy stabilisation at low magnetic flux. Moreover, two types of antiferromagnetic transition versus the flux occurring for a correlation term larger than a critical one have been observed, i.e. the likelihood of a charge excitation before the antiferromagnetic transition. Finally, a comparison between the results obtained from the exact diagonalisation and the Gutzwiller method has been carried out, leading to a suggested modification of the Gutzwiller approach in order to improve it. Received 23 June 1999 and Received in final form 28 July 2000     

Dissociation channels of silver bromide cluster Ag<Subscript>2</Subscript>Br,silver cluster Ag<Subscript>3</Subscript> and their ions studied by using alkali metal target

Various dissociation channels of silver bromide cluster ion Ag₂Br⁺ and silver cluster ion Ag₃ ⁺ were observed in high-energy collisionally-activated dissociation (CAD) using a Cs target. The fragment patterns of the high-energy CAD were compared with those of the metastable dissociation and low-energy CAD. The difference in the fragment patterns between the high-energy CAD and the other dissociation methods was explained in terms of the internal energy distributions. The dissociation mechanisms of neutral silver bromide cluster Ag₂Br and silver cluster Ag₃ were also investigated by charge inversion mass spectrometry using the Cs target. While the fragment ions AgBr^- and Ag₂ ^- were dominantly observed in the charge inversion spectrum of Ag₂Br⁺, the undissociated ion Ag₃ ^- was observed as a predominant peak in the case of Ag₃ ⁺. The dissociation behavior of Ag₂Br^* can be explained on the basis of the calculated thermochemical data. Contrary to this, the predominant existence of the undissociated Ag₃ ^- cannot be explained by the reported thermochemical data. The existence of undissociated Ag₃ ^- suggests that the dissociation barrier is higher than the internal energy of Ag₃ ^* (theoretical: 1.03 eV, experimental: 2.31 eV) estimated from the ionization potentials of Ag₃ and Cs.     

C 1s core photoemission of C60 and C48N12

We make a theoretical study of the shake-up of the 1s photoemission of C₆₀. The method takes into account the N-body reactions of the π and σ electrons which appear during the formation of the photoemission hole on one carbon atom. We analyze the origin of the satellite in the spectra due to transitions between N-body states. Our calculation shows that the satellite spectra is essentially given by N-body transitions which involve the creation of one or two electron-hole pairs. The method has been applied also to C₄₈N₁₂. The situation is more complex. The spectra of the two most stable species have been investigated. Moreover the influence on the spectra of the position of the hole created on the carbon atom in C₄₈N₁₂ has been examined (all the carbon positions are not equivalent for some isomers).     

Radiative cooling of fullerene anions in a storage ring

Thermionic emission from hot fullerene anions, C_N ^-, has been measured in an electrostatic storage ring for even N values from 36 to 96. The decay is quenched by radiative cooling and hence the observations give information on the intensity of thermal radiation from fullerenes. The experiments are analysed by comparison with a simulation which includes the quantisation of photon energy and the statistics of emission. Experiments with heating of the molecules with a laser beam confirm the interpretation of the observations in terms of radiative cooling and give an independent estimate of the cooling rate for C₆₀ ^-. The measured cooling rates agree in general within a factor of two with the prediction from a classical dielectric model of a thermal radiation intensity of ∼ 300 eV/s for C₆₀ at 1 400 K, scaling approximately with the 6th power of the temperature and with the number of atoms in the molecule. Received 12 March 2001 and Received in final form 12 June 2001     

Electron multiplicity in slow collisions of Ar ions with C

Electron capture by Ar⁸⁺ in collisions with C₆₀ fullerene has been investigated using coincident measurements of the number n of ejected electrons, the mass and charge of multicharged Cr+ ₆₀ recoil ions and their fragments Ci+ m and the final charge state of outgoing projectiles Ar(8-s)+ (). The number of captured electrons r is the sum of the numbers of stabilized and emitted electrons: r = n + s. The ratio n / s decreases by a factor three with s increasing from 1 to 7 showing that the multiply excited states populated by capture of a large number of electrons are rather stable against auto-ionisation. Each kinetic energy spectrum of Ar⁺ and Ar²⁺ projectiles is composed of two peaks which we attribute to collisions “inside” and “outside” the C₆₀ cage. The measured energy shift of the projectile keV is consistent with the corresponding energy loss keV in a carbon foil with an equivalent thickness. Inside collisions are characterized by a strong dissociation of recoil ions into light monocharged fragments and by a high multiplicity of ejected electrons. Received: 25 March 1998 / Received in final form and Accepted: 9 June 1998     

Tight-binding study of structural and electronic properties of silver clusters

Tight-binding model is developed to study the structural and electronic properties of silver clusters. The ground state structures of Ag clusters up to 21 atoms are optimized by molecular dynamics-based genetic algorithm. The results on small Ag_n clusters (n = 3-9) are comparable to ab initio calculations. The size dependence of electronic properties such as density of states, s-d band separation, HOMO-LUMO gap, and ionization potentials are discussed. Magic number behavior at Ag₂, Ag₈, Ag₁₄, Ag₁₈, Ag₂₀ is obtained, in agreement with the prediction of electronic ellipsoid shell model. We suggest that both the electronic and geometrical effect play significant role in the coinage metal clusters. Received 7 August 2000     

Doubly charged clusters - neutral atom charge transfer: the role of the Coulombic repulsion

We have studied experimentally the collisional charge transfer between a neutral atom and a multicharged metal-atom cluster. The charge transfer cross section measured for Na ₃₁ ^{+ +} + Cs is in the range of 400 ?². The time-of-flight mass analysis of the singly charged collision products demonstrates that an energy of about 0.5 eV is deposited in the cluster fragment during the charge transfer collision. This effect can be interpreted as a charge transfer to an excited state of the metal cluster. The measured cross section for Na ₃₁ ^{+ +} + Cs is larger than the one for Na ₃₁ ⁺ + Cs collisions. This difference between these two systems is due to the existence, for the first one, of a Coulombic repulsion term in the collision output channel. Received 24 October 2000     

Positronium formation cross-sections in the ground and excited states ( levels) in an -He atom collision

The positronium formation cross-sections in the ground and excited n=2 levels have been studied in an -He atom collision in the framework of eikonal approximation. Both the differential and total formation cross-sections have been investigated in the intermediate- and high-energy regime. Present eikonal results are found to differ appreciably from the corresponding first Born values even at very high incident energies. The total cross-section results have been compared with available experiments due to different groups as well as with other existing theoretical results. Received: 20 July 1998 / Received in final form: 5 January 1999     

Non-collinear magnetic moments of seven-atom Cr, Mn and Fe clusters

The non-collinearity of magnetic moments of pentagonal bipyramid Cr₇, Mn₇ and Fe₇ clusters is discussed. The magnetic moments are calculated by the discrete variational non-collinear spin-density functional method. For the Cr₇ cluster, a coplanar magnetic arrangement appears at the large interatomic distance. With decreasing the interatomic distance, the coplanar arrangement changes to the parallel arrangement with a small absolute magnetic moment. For the Mn₇ cluster, the magnetic arrangement changes from coplanar to antiparallel with decreasing the interatomic distance. Also for the Fe₇ cluster, some coplanar magnetic moments appear at the interatomic distance of 2.23 ?. In these coplanar magnetic arrangements, the magnetic moment at the basal site of the pentagon rotates with a step of 144 degrees for the Cr₇ clusters and 72 degrees for the Mn₇ and Fe₇ clusters. Received 30 November 2000     

Effect of melting on ionization potential of sodium clusters

The effect of melting transition on the ionization potential has been studied for sodium clusters with 40, 55, 142, and 147 atoms, using ab initio and classical molecular dynamics. Classical and ab initio simulations were performed to determine the ionization potential of Na₁₄₂ and Na₁₄₇ for solid, partly melted, and liquid structures. The results reveal no correlation between the vertical ionization potential and the degree of surface disorder, melting, or the total energy of the cluster obtained with the ab initio method. However, in the case of 40 and 55 atom clusters, the ionization potential seems to decrease when the cluster melts. Received 1st November 2002 Published online 24 April 2003 RID="a" ID="a"e-mail: ar@phys.jyu.fi     

Metallic evolution of small magnesium clusters

Structural and electronic properties of small magnesium clusters (N≤13) are studied using a first-principles simulation method in conjunction with the density functional theory and generalized gradient correction approximation for the exchange-correlation energy functional. It is observed that the onset of metallization of magnesium clusters is hard to assign since both the s-p hybridization and the energy gap between the valence and conduction bands do not evolve rapidly towards the known bulk properties. Instead these quantities show a slow and nonmonotonic evolution. Received 15 November 2000     

Observation of multiply charged silver-cluster anions

Singly charged silver-cluster anions are produced in a laser vaporization source and transferred into a Penning trap. After size selection the clusters are subjected to an electron bath in the trap, which results in the attachment of further electrons. The relative abundance of dianions or trianions as a function of the clusters' size is analyzed by time-of-flight mass spectrometry. Silver-cluster dianions are observed for sizes n≥ 24 and trianions for n > 100. In addition, a detailed study of the cluster sizes 24 ?n? 60 shows a pronounced resistance to electron attachment for singly charged anions Ag_n ^- with a closed electronic shell, in particular Ag₂₉ ^-, Ag₃₃ ^-, and Ag₃₉ ^-. Both the threshold size for the observation of dianionic silver clusters and the shell effects in the production yield correlate favorably with previous theoretical investigations of the respective electron affinities. Received 24 November 2000