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1.
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
2.
M. Bertolus V. Brenner P. Millié 《The European Physical Journal D - Atomic, Molecular, Optical and Plasma Physics》2000,11(3):387-394
An ab initio study of the Nan(OH)n, Nan(OH)n-1
+, Agn(OH)n, and Agn(OH)n-1
+ clusters with n up to four is presented. The results of this study show that, in accordance with experimental observations, the sodium hydroxide
clusters are almost purely ionic, while the Ag-O bond exhibits a significant covalent character. The perturbation caused by
the non-spherical OH- group relatively to an atomic anion, as well as the influence on structures and energies of the covalent character of the
metal-oxygen bond are determined. The appearance of metal-metal bonds in the silver hydroxide clusters is also discussed.
Finally, the theoretical results obtained on the Na-OH clusters are compared to experimental results available on the dissociation
of the Nan(OH)n-1
+ clusters.
Received 9 August 1999 and Received in final form 1st December 1999 相似文献
3.
A. Aguado L.M. Molina J.M. López J.A. Alonso 《The European Physical Journal D - Atomic, Molecular, Optical and Plasma Physics》2001,15(2):221-227
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 相似文献
4.
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
5.
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
6.
Systematics of the melting transition for sodium clusters with 40-355 atoms has been studied with both ab initio and semiclassical molecular dynamics simulations. The melting temperatures obtained with an ab initio method for Na55 + and Na93 + correlate well with the experimental results. The semiclassically determined melting temperatures show similarities with the experimentally determined ones in the size region from 55 to 93 and near size 142, and the latent heat in the size region from 55 to 139, but not elsewhere in the size region studied. This indicates that the nonmonotonical melting behavior observed experimentally cannot be fully explained by geometrical effects. The semiclassically determined melting temperature and the latent heat correlate quite well, indicating that they respond similarly to changes in cluster geometry and size. Similarly, the binding energy per atom seems to correlate with the melting temperature and the latent heat of fusion.Received: 30 October 2003, Published online: 20 January 2004PACS:
36.40.Ei Phase transitions in clusters 相似文献
7.
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
8.
F. Fehrer P. M. Dinh M. Bär P.-G. Reinhard E. Suraud 《The European Physical Journal D - Atomic, Molecular, Optical and Plasma Physics》2007,45(3):447-458
We investigate the dynamical evolution of a Na8 cluster embedded in Ar matrices of various sizes from N=30 to 1048.
The system is excited by an intense short laser pulse leading to high
ionization stages.We analyze the subsequent highly non-linear motion of cluster and Ar environment in terms of trajectories,
shapes, and energy flow.
The most prominent effects are: temporary stabilization of high charge states for several ps, sudden stopping of the Coulomb
explosion of the embedded Na8
clusters associated with an extremely fast energy transfer to the Ar
matrix, fast distribution of energy throughout the Ar layers by a sound wave.
Other ionic-atomic transfer and relaxation processes proceed at slower
scale of few ps. The electron cloud is almost thermally decoupled
from ions and thermalizes far beyond the ps scale. 相似文献
9.
A. Heidenreich I. Last J. Jortner 《The European Physical Journal D - Atomic, Molecular, Optical and Plasma Physics》2008,46(1):195-202
We present a theoretical and computational study of the properties and the
response of the nanoplasma and of outer ionization in Xen clusters (n =
55–2171, initial cluster radius R0 = 8.7–31.0 ?) driven by
ultraintense near-infrared laser fields (peak intensity IM = 1015–1020 Wcm-2, temporal pulse length τ= 10–100 fs, and frequency ν= 0.35 fs-1). The positively charged high-energy nanoplasma produced by inner ionization nearly follows the oscillations of
the fs laser pulse and can either be persistent (at lower intensities of IM = 1015–1016 Wcm-2 and/or for larger cluster sizes, where the electron energy distribution is nearly thermal) or transient (at higher intensities
of IM = 1018–1020 Wcm-2 and/or for smaller cluster sizes). The nanoplasma is depleted by outer ionization that was semiquantitatively described by
the cluster barrier suppression electrostatic model, which accounts for the cluster size, laser intensity and pulse length
dependence of the outer ionization yield. The electrostatic model was further utilized for estimates of the laser intensity
and pulse
width dependence of the border radius R0
(I) for the attainment of complete outer ionization at
,
while at R0 > R0
(I) a persistent nanoplasma prevails. R0
(I)
establishes an interrelationship between electron dynamics and nuclear Coulomb explosion dynamics in ultraintense
laser-cluster interactions. 相似文献
10.
V. Boutou A.R. Allouche F. Spiegelmann J. Chevaleyre M. Aubert Frécon 《The European Physical Journal D - Atomic, Molecular, Optical and Plasma Physics》1998,2(1):63-73
The geometrical structure of ground state Ban clusters (n
=2-14) has been predicted from various types of calculations including two ab initio approaches used for the smaller sizes namely HF+MP2(
n
=2-6), DFT (LSDA)(
n
=2-6, 9) and one model approach HF+pairwise dispersion used for all sizes investigated here. The lowest energy configurations
as well as some isomers have been investigated. The sizes n
=4, 7 and 13 are predicted to be the relatively more stable ones and they correspond to the three compact structures: the tetrahedron,
the pentagonal bipyramid and the icosahedron. The growth behavior from Ba7 to Ba13 appears to be characterized by the addition of atoms around a pentagonal bipyramid leading to the icosahedral structure of
Ba13 which is consistent with the observed size-distribution of barium clusters. Values for vertical ionization potentials calculated
for n
=2-5 at the CI level are seen to be in quite good agreement with recent measures.
Received: 14 May 1997 / Received in final form: 2 February 1998 / Accepted: 27 February 1998 相似文献
11.
K. A. MCLAUCHLAN 《Molecular physics》2013,111(1):9-10
A new flexible atomic and polarizable potential for water simulation is validated and applied to the study of small clusters of water molecules: (H2O) n , n = 4, 6 and 8. The low-energy equilibrium structures obtained are in good agreement with ab initio calculations. Vibrational frequencies are calculated by normal-mode analysis and are in semiquantitative agreement with ab initio data. Binding energies and dipole moments are also satisfactorily reproduced, despite the limited number of parameters of the potential. 相似文献
12.
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
13.
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
14.
采用分子动力学方法及淬火技术,结合Gupta势和Sutton-Chen势,模拟研究了包含13,14,55,56,147及148个原子数的铱团簇的熔化行为. 结果表明,Gupta势和Sutton-Chen势对所研究的Ir团簇的基态几何结构和熔化行为给出了基本一致的描述:两种不同势给出了完全相同的基态几何结构;两种势给出的Ir团簇熔点及预熔化区间随团簇尺寸的变化关系基本一致;对于小Irn团簇(n=13,14)两类势均表现出比热峰值相对于均方根键长涨落饱和值滞后的现象. 但是
关键词:
铱团簇
分子动力学
Gupta势和Sutton-Chen势
熔化 相似文献
15.
M. Nakamura R.-J. Tarento P. Joyes 《The European Physical Journal D - Atomic, Molecular, Optical and Plasma Physics》2003,24(1-3):169-172
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. 相似文献
16.
G. Durand F. Spiegelman A. R. Allouche 《The European Physical Journal D - Atomic, Molecular, Optical and Plasma Physics》2003,24(1-3):19-22
Recently, electric susceptibilities of
NanFn-1 clusters
have been measured by deflecting a molecular beam in an
inhomogeneous electric field. The analysis of the deflection of
a cluster by the electric field needs the calculation of the
electric properties. We present the calculation of the static
anisotropic and average dipolar polarizabilities within a model
in which the
NanFn-1 clusters (
2
n
23)
are treated as one electron embedded in the field of
n ions
Na+ and of n
- 1
ions F-. The accuracy of the results
is evaluated and discussed on small clusters (n
5)
in comparison with ab initio
calculations. The relationship between the polarizabilities, the
electronic localization and the geometric structure is
discussed. Received 10 September 2002 Published online 3 July
2003 相似文献
17.
C. Coudray G. Blaise M.J. Malliavin 《The European Physical Journal D - Atomic, Molecular, Optical and Plasma Physics》2000,11(1):127-136
With the help of ab initio methods the clusters [(MgO)13Mg]
Q+
are simulated for Q = 0, 1, 2. Then, vacancy clusters [(MgO)12Mg2]
Q+
obtained by removing one oxygen atom are computed for Q running from 0 to 4. These clusters exhibit a slight sphericity and generally shorter interatomic distances than in the crystal.
The electronic densities variations are studied in function of Q. In particular, it is observed that the electronic density in the oxygen vacancy goes to a maximum when Q = 2. The ionisation potentials vary from approximately 4 to 14 eV when Q varies from 0 to 3, with a more rapid increase from Q = 1 to Q = 2. The stability study of vacancy clusters show that they experience a phase transition when their charge becomes equal
to 2, in accordance with the features mentioned above.
Received 14 September 1999 and Received in final form 2 December 1999 相似文献
18.
F.O. Talbot J.P. Simons 《The European Physical Journal D - Atomic, Molecular, Optical and Plasma Physics》2002,20(3):389-398
Mass-resolved resonant two photon ionisation (R2PI) and infrared ion dip spectra have been recorded for 4-phenylimidazole
(4PI) and its singly and multiply hydrated clusters 4PI(H2O)n = 0 - 4, under supersonic expansion conditions. In the case of 4PI(H2O)0,1, it has also been possible to record infrared spectra in both the ground (S0) and excited (S1) states. Combining the experimental data with the results of ab initio calculations has led to the structural assignment of each cluster. In each case, the water molecules bind primarily to the
NH site of the imidazole ring. Clusters with n≥ 2 incorporate linear water chains, in which the proton donating terminus bridges either to the π-electron system (n = 2) or to the >N: atom site (n = 3, 4) on the imidazole ring. Despite the creation of a “water wire”, connecting the donor and acceptor sites of imidazole,
there is no evidence of proton transfer in either the ground or excited state.
Received 20 December 2001 Published online 13 September 2002 相似文献
19.
Metastable fragmentation of silver bromide clusters 总被引:2,自引:0,他引:2
J.-M. L'Hermite F. Rabilloud L. Marcou P. Labastie 《The European Physical Journal D - Atomic, Molecular, Optical and Plasma Physics》2001,14(3):323-330
The abundance spectra and the fragmentation channels of silver bromide clusters have been measured and analyzed. The most
abundant species are AgnBrn - 1
+ and AgnBrn + 1
- and Ag14Br13
+ is a magic number, revealing their ionic nature. However, some features depart from what is generally observed for alkali-halide
ionic clusters. From a certain size, AgnBrn - 1
+ is no more the main series, and AgnBr n - 2, 3
+ series become almost as important. The fast fragmentation induced by a UV laser makes the cations lose more bromine than
silver ions and lead to more silver-rich clusters. Negative ions mass spectra contain also species with more silver atoms
than required by stoichiometry. We have investigated the metastable fragmentation of the cations using a new experimental
method. The large majority of the cations release mainly a neutral Ag3Br3 cluster. These decay channels are in full agreement with our recent ab initio DFT calculations, which show that Ag+-Ag+ repulsion is reduced due to a globally attractive interaction of their d orbitals. This effect leads to a particularly stable trimer (AgBr)3 and to quasi-planar cyclic structures of (AgBr)n clusters up to n = 6. We have shown that these two features may be extended to other silver halides, to silver hydroxides (AgOH)n, and to cuprous halide compounds.
Received 9 November 2000 and Received in final form 25 January 2001 相似文献
20.
L. Kronik R. Fromherz E. Ko G. Ganteför J. R. Chelikowsky 《The European Physical Journal D - Atomic, Molecular, Optical and Plasma Physics》2003,24(1-3):33-36
We compare experimentally measured and
ab initio computed
photoelectron spectra of negatively charged deuterated silicon
clusters (
, 4m10, 0n2) produced in a plasma environment.
Based on this comparison, we discuss the kinetics and
thermodynamics of the cluster formation and the effect of
deuterium on the geometrical and electronic structure of the
clusters. 相似文献