共查询到20条相似文献,搜索用时 46 毫秒
1.
J. Zhao Y. Luo G. Wang 《The European Physical Journal D - Atomic, Molecular, Optical and Plasma Physics》2001,14(3):309-316
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 Agn 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 相似文献
2.
C. Yannouleas U. Landman A. Herlert L. Schweikhard 《The European Physical Journal D - Atomic, Molecular, Optical and Plasma Physics》2001,16(1):81-85
Using Penning-trap experiments and a shell-correction method incorporating ellipsoidal shape deformations, we investigate
the formation and stability patterns of trianionic gold clusters. Theory and experiment are in remarkable agreement concerning
appearance sizes and electronic shell effects. In contrast to multiply cationic clusters, decay of the trianionic gold clusters
occurs primarily via electron autodetachment and tunneling through a Coulomb barrier, rather than via fission.
Received 9 January 2001 相似文献
3.
A. Herlert L. Schweikhard M. Vogel 《The European Physical Journal D - Atomic, Molecular, Optical and Plasma Physics》2001,16(1):65-68
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 Agn
- 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 相似文献
4.
A. Rytkönen M. Manninen 《The European Physical Journal D - Atomic, Molecular, Optical and Plasma Physics》2003,23(3):351-357
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 相似文献
5.
G. Chen Z.F. Liu X.G. Gong 《The European Physical Journal D - Atomic, Molecular, Optical and Plasma Physics》2001,16(1):33-36
We have studied the atomic structure and the electronic properties of Ban clusters by the ab initio molecular dynamics method. We find that a structural transition to the bulk-like structure begins at Ba9 cluster, and the structures of the clusters are transferred to be icosahedral-like around n
= 13. The relatively high stability for Ba4, Ba10 and Ba13 clusters are observed.
Received 1st December 2000 相似文献
6.
Systematic study of small BN clusters 总被引:2,自引:0,他引:2
S. Guerini P. Piquini 《The European Physical Journal D - Atomic, Molecular, Optical and Plasma Physics》2001,16(1):17-20
We performed a systematic investigation of the small BxNy (x + y? 6) clusters using the ab initio Hartree-Fock scheme plus second-order perturbation theory. The nature of the potential energy surface extrema are analyzed
through analytical total energy second derivatives. Ionization potentials, binding energies and the stability against some
possible reaction mechanisms are calculated. Based on these results we propose that the growing process for these clusters
is mainly due to the successive incorporation of BN molecules. A discussion of some mass spectrometry experimental results
is also presented.
Received 2 October 2000 相似文献
7.
V. O. Nesterenko W. Kleinig P. -G. Reinhard 《The European Physical Journal D - Atomic, Molecular, Optical and Plasma Physics》2002,19(1):57-64
Recent experimental data on the dipole plasmon in axial sodium clusters Na N + with 11 ≤ N ≤ 57 are analyzed within a self-consistent separable random-phase approximation (SRPA) based on the deformed Konh-Sham functional. Good agreement with the data is achieved. The calculations show that, while in light clusters plasmon properties (gross structure and width) are determined mainly by deformation splitting, in medium clusters with N τ 50 the Landau fragmentation becomes decisive. Moreover, in medium clusters shape isomers come to play with contributions to the plasmon comparable with the ground state one. As a result, commonly used methods of the experimental analysis of cluster deformation become useless and correct treatment of cluster shape requires microscopic calculations. 相似文献
8.
K. Ohshimo H. Tsunoyama F. Misaizu K. Ohno 《The European Physical Journal D - Atomic, Molecular, Optical and Plasma Physics》2001,16(1):107-110
Intracluster electron transfer and oligomerization reaction were investigated by mass spectrometry of clusters of alkali metal
atom (M) with acrylonitrile (AN; CH2=CHCN). In the photoionization mass spectra of M(AN)n, magic numbers were clearly observed at n = 3k (k = 1-4 for M = Na and K, k = 1 for M = Li). The results of photodissociation of neutral K(AN)n indicate that the n = 3 cluster has an anomalous stability relative to other sizes of clusters. The C=C bond in vinyl molecules is also found
to be necessary to form the magic numbers by measuring the photoionization mass spectrum of K atom with propionitrile. These
results strongly support the intracluster anionic oligomerization reaction initiated by electron transfer from the alkali
atom. The quantum chemical calculations have revealed that the evaporation induced by excess energy generated by intracluster
oligomerization is important to form the magic numbers in the present clusters.
Received 29 November 2000 相似文献
9.
T. Döppner Th. Diederich J. Tiggesbäumker K.-H. Meiwes-Broer 《The European Physical Journal D - Atomic, Molecular, Optical and Plasma Physics》2001,16(1):13-16
Magnesium clusters grown in helium droplets and ionized with femtosecond laser pulses have been studied by high resolution
mass spectrometry. For moderate laser intensities the abundance spectra show characteristic features indicating electronic
shell effects. Compared to clusters of s1-electron metals additional shell closures appear resulting from an electron rearrangement. Irradiation with higher laser
intensities leads to a decomposition of the magnesium clusters into atomic ions. Due to charge exchange with the surrounding
helium matrix mainly singly and doubly charged magnesium ions remain. In addition, the occurrence of MgHeN
+-complexes is observed. Their abundance depends on the shape of the laser field, i.e. the laser width and the optical delay when applying the pump-probe technique.
Received 2 January 2001 相似文献
10.
R.J. Tarento P. Joyes J. van de Walle 《The European Physical Journal D - Atomic, Molecular, Optical and Plasma Physics》2001,13(3):355-360
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 相似文献
11.
J. Akola A. Rytkönen H. Häkkinen M. Manninen 《The European Physical Journal D - Atomic, Molecular, Optical and Plasma Physics》2000,8(1):93-99
The ionization potential of sodium clusters () at a finite temperature is studied using density functional theory and ab initio molecular dynamics. The threshold regions of the photoionization efficiency curves are deduced from the integrated IP distributions,
which are obtained from the energy eigenvalues of the highest occupied Kohn-Sham states during molecular dynamics by applying
a theoretically well-defined shift. The calculated ionization potentials are directly compared to the experimental values.
The energetically best geometry of Na55 is found to be a slightly distorted icosahedron.
Received 16 April 1999 and Received in final form 6 July 1999 相似文献
12.
P. Parneix 《The European Physical Journal D - Atomic, Molecular, Optical and Plasma Physics》2003,23(3):375-383
The isomerization and evaporation processes in the neutral homogeneous (CH3CN)n molecular clusters (n
= 2-7) have been investigated using classical molecular dynamics simulations. The evaporation rate constants and the kinetic energy
release in the dissociation have been analysed as a function of the cluster size and as a function of the internal energy
in the parent cluster. The competition between monomer and dimer ejections has been also carefully studied. All the dynamical
properties in these dissociative processes have been discussed in relation to the static properties of the clusters involved
in the dissociation and also in relation to the solid-liquid like transition which appears in these homogeneous molecular
clusters.
Received 19 November 2002 / Received in final form 5 February 2003 Published online 29 April 2003
RID="a"
ID="a"e-mail: pascal.parneix@ppm.u-psud.fr
RID="b"
ID="b"Laboratoire associé à l'université Paris-Sud. 相似文献
13.
M. Vogel K. Hansen A. Herlert L. Schweikhard 《The European Physical Journal D - Atomic, Molecular, Optical and Plasma Physics》2001,16(1):73-76
The decay pathway competition between monomer and dimer evaporation of photoexcited cluster ions Au
+
n, n = 2-27, has been investigated by photodissociation of size-selected gold clusters stored in a Penning trap. For n > 6 the two decay pathways are distinguished by their experimental signature in time-resolved measurements of the dissociation.
For the smaller clusters, simple fragment spectra were used. As in the case of the other copper-group elements, even-numbered
gold cluster ions decay exclusively by monomer evaporation, irrespective of their size. For small odd-size gold clusters,
dimer evaporation is a competitive alternative, and the smaller the odd-sized clusters, the more likely they decay by dimer
evaporation. In this respect, Au
+
9 shows an anomalous behavior, as it is less likely to evaporate dimers than its two odd-numbered neighbors, Au
+
7 and Au
+
11. This nonamer anomaly is typical for copper-group cluster ions M
+
9 (M = Cu, Ag, Au) and a similar behavior is found in the anionic heptamers M
-
7. It is discussed in terms of the well-known electronic shell closing at n
e = 8 atomic valence electrons.
Received 2 November 2000 相似文献
14.
C. Bobbert S. Schütte C. Steinbach U. Buck 《The European Physical Journal D - Atomic, Molecular, Optical and Plasma Physics》2002,19(2):183-192
The interaction of large ammonia and water clusters in the size range from <n> = 10 to 3 400 with electrons is investigated in a reflectron time-of-flight mass spectrometer. The clusters are generated
in adiabatic expansions through conical nozzles and are nearly fragmentation free detected by single photon ionization after
they have been doped by one sodium atom. For ammonia also the (1+1) resonance enhanced two photon ionization through the state with v = 6 operates similarly. In this way reliable size distributions of the neutral clusters are obtained which are analyzed in
terms of a modified scaling law of the Hagena type [Surf. Sci. 106, 101 (1981)]. In contrast, using electron impact ionization, the clusters are strongly fragmented when varying the electron
energy between 150 and 1 500 eV. The number of evaporated molecules depends on the cluster size and the energy dependence
follows that of the stopping power of the solid material. Therefore we attribute the operating mechanism to that which is
also responsible for the electronic sputtering of solid matter. The yields, however, are orders of magnitude larger for clusters
than for the solid. This result is a consequence of the finite dimensions of the clusters which cannot accommodate the released
energy.
Received 21 November 2001 相似文献
15.
S. Varga K. Bolton H. Grönbeck A. Snis A. Rosén B. Fricke 《The European Physical Journal D - Atomic, Molecular, Optical and Plasma Physics》2001,16(1):29-32
We present recent theoretical results for the V3 and Au4 clusters. Calculations of the V3 doublet system indicate that the 6-311+G(d) basis set is sufficiently flexible to provide reliable minimum energy structures
and vibrational frequencies, that these structures and frequencies are insensitive to spin contamination of the wave function
when the BPW91 functional is used, and that changing to the B3LYP functional may result in very different structures and frequencies.
A computationally less expensive scalar relativistic treatment of Au4 clusters gives structural properties that are in good agreement with those obtained using a four-component method.
Received 30 November 2000 相似文献
16.
I. L. Garzón M. R. Beltrán G. González I. Guterrez-González K. Michaelian J. A. Reyes-Nava J. I. Rodrguez-Hernández 《The European Physical Journal D - Atomic, Molecular, Optical and Plasma Physics》2003,24(1-3):105-109
Theoretical and experimental information on the shape and
morphology of bare and passivated gold clusters is fundamental
to predict and understand their electronic, optical, and other
physical and chemical properties. An effective theoretical
approach to determine the lowest-energy configuration (global
minimum) and the structures of low energy isomers (local minima)
of clusters is to combine genetic algorithms and many-body
potentials (to perform global structural optimizations), and
first-principles density functional theory (to confirm the
stability and energy ordering of the local minima). The main
trend emerging from structural optimizations of bare Au clusters
in the size range of 12-212 atoms indicates that many
topologically interesting low-symmetry, disordered structures
exist with energy near or below the lowest-energy ordered
isomer. For example, chiral structures have been obtained as the
lowest-energy isomers of bare Au28 and
Au55 clusters, whereas in the size-range
of 75-212 atoms, defective Marks decahedral structures are
nearly degenerate in energy with the ordered symmetrical
isomers. For methylthiol-passivated gold nanoclusters
[Au28(SCH3)16
and
Au38(SCH3)24],
density functional structural relaxations have shown that the
ligands are not only playing the role of passivating molecules,
but their effect is strong enough to distort the metal cluster
structure. In this work, a theoretical approach to characterize
and quantify chirality in clusters, based on the Hausdorff
chirality measure, is described. After calculating the index of
chirality in bare and passivated gold clusters, it is found that
the thiol monolayer induces or increases the degree of chirality
of the metallic core. We also report simulated high-resolution
transmission electron microscopy (HRTEM) images which show that
defects in decahedral gold nanoclusters, with size between 1-2
nm, can be detected using currently available experimental HRTEM
techniques. 相似文献
17.
V. Kasperovich K. Wong G. Tikhonov V.V. Kresin 《The European Physical Journal D - Atomic, Molecular, Optical and Plasma Physics》2001,16(1):99-102
An analysis of integral cross sections for slow electron collisions with neutral sodium clusters and nanoparticles reveals
that, in addition to an effective negative ion formation channel, there exists a strong inelastic threshold-type process which
appears above a collision energy of 1-1.3 eV. We show that it can be plausibly associated with the onset of direct electron-induced
cluster fragmentation. This result highlights the importance of understanding the dynamics of electron-vibrational energy
transfer in nanoclusters, including the relative probability of direct vs. statistical energy transfer.
Received 24 November 2000 相似文献
18.
J.U. Andersen C. Gottrup K. Hansen P. Hvelplund M.O. Larsson 《The European Physical Journal D - Atomic, Molecular, Optical and Plasma Physics》2001,17(2):189-204
Thermionic emission from hot fullerene anions, CN
-, 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 相似文献
19.
P. Farmanara H.-H. Ritze V. Stert W. Radloff I.V. Hertel 《The European Physical Journal D - Atomic, Molecular, Optical and Plasma Physics》2002,19(2):193-209
Neutral ammonia clusters (NH3)m are photo-excited to the electronic state by a deep UV femtosecond laser pump pulse. Within a few hundred femtoseconds a significant fraction of the clusters
rearrange to form an H-transfer state (NH3)m-2NH4(3s)NH2 with the subunit NH4 in its 3s electronic ground state. This state is then electronically excited by a time-delayed infrared control pulse of variable wavelength.
Finally, a third (probe) pulse in the UV ionizes the clusters for detection. The lifetime of the excited (NH3)m-2NH4(3p)NH2 states is found to vary between 2.7 and 0.13 ps depending on cluster size and excitation energy. It increases drastically
upon deuteration. The corresponding cluster size-dependent photoelectron spectra allow us to disentangle the underlying energetics
of the excitation and ionization process and reveal additional processes, such as nonresonant ionization or dissociative ionization.
The experimental findings suggest that the excited H-transfer ammonia complexes with m > 2 are deactivated by an internal conversion process back to the electronically lowest H-transfer state followed by fast
dissociation.
Received 22 September 2001 and Received in final form 31 January 2002 相似文献
20.
K. Hashimoto M. Okamoto K. Takayanagi 《The European Physical Journal D - Atomic, Molecular, Optical and Plasma Physics》1998,2(1):75-78
The stability of neutral, singly and multiply ionized silicon clusters, (N
= 2-7, M
= 0, , , ), has been investigated using an ab initio density functional method. We show that the fragmentation effect significantly affects the structure of mass-spectra of multiply
ionized silicon clusters. For clusters, the clusters with a large fragmentation energy are found to correspond to the high peaks at N = 4 and 6 in mass-spectra. For clusters, a peak at N = 5 in mass-spectra has been predicted to be especially high.
Received: 9 June 1997 / Revised: 8 January 1998 / Accepted: 25 February 1998 相似文献