共查询到20条相似文献,搜索用时 20 毫秒
1.
H. Failache S. Saltiel M. Fichet D. Bloch M. Ducloy 《The European Physical Journal D - Atomic, Molecular, Optical and Plasma Physics》2003,23(2):237-255
We present a detailed experimental study of the evaluation of the van der Waals (vW) atom-surface interaction for high-lying
excited states of alkali-metal atoms (Cs and Rb), notably when they couple resonantly with a surface-polariton mode of the
neighbouring dielectric surface. This report extends our initial observation [Phys. Rev. Lett. 83, 5467 (1999)] of a vW repulsion between Cs(6D3/2) and a sapphire surface. The experiment is based upon FM selective reflection spectroscopy, on a transition reaching a high-lying
state from a resonance level, that has been thermally pumped by an initial one-photon step. Along with a strong vW repulsion
fitted with a blue lineshift, -160±25 kHz μm3 for Cs(6D3/2) in front of a sapphire surface (with a perpendicular c-axis), we demonstrate a weaker vW repulsion (-32±5 kHz μm3) for Cs(6D3/2) in front of a YAG surface, as due to a similar resonant coupling at 12 μm between a virtual atomic emission (6D3/2-7P1/2) and the surface polariton modes. A resonant behaviour of Rb(6D5/2) in front of a sapphire surface exists also because of analogous decay channels in the 12 μm range. Finally, one demonstrates
that fused silica, nonresonant for a virtual transition in the 12 μm range and hence weakly attracting for Cs(6D3/2), exhibits a resonant behaviour for Cs(9S1/2) as due to its surface polariton resonance in the 8-9 μm range. The limiting factors that affect both the accuracy of the
theoretical prediction, and that of the fitting method applied to the experimental data, are discussed in the conclusion.
Received 16 January 2003 / Received in final form 25 March 2003 Published online 5 May 2003 相似文献
2.
M.-P. Gorza M. Ducloy 《The European Physical Journal D - Atomic, Molecular, Optical and Plasma Physics》2006,40(3):343-356
The long-range interactions between an atomic system in an arbitrary energy
level and dispersive surfaces in thermal equilibrium at non-zero temperature
are revisited within the framework of the quantum-mechanical linear response
theory, using generalized susceptibilities for both atom and electromagnetic
field. After defining the observables of interest, one presents a general
analysis of the atomic level shift valid for any number and form of
dielectric surfaces. It is shown that, at zero temperature, one recovers
well-known results previously obtained in the linear response regime. The
case of a plane dispersive surface is elaborated on in the non-retarded
regime. Calculations are given in detail for a dielectric surface exhibiting
a single polariton resonance. Theoretical predictions are presented within a
physical viewpoint allowing one to discriminate between the various
interaction processes: on one hand, the level shift induced by non-resonant
quantum fluctuations, on the other hand, two potentially resonant
atom-surface couplings. The first resonant process appears for excited-state
atoms and originates in an atomic de-excitation channel resonantly coupled
to the surface polariton mode. It exists also at zero temperature, and has
been studied and observed previously. The second physical process, which
exists at non-zero temperature only, corresponds to the reverse process in
which a thermal quantum excitation of a surface polariton resonantly couples
to an atomic absorption channel. This novel phenomenon is predicted as well
for a ground state atom, and can turn the ordinary long-range van der Waals
attraction of atoms into a surface repulsion at increasing temperatures.
This opens the way to the control and engineering of the sign and amplitude
of van der Waals forces via surface temperature adjustment. 相似文献
3.
G. Durand F. Spiegelmann 《The European Physical Journal D - Atomic, Molecular, Optical and Plasma Physics》2001,13(2):237-243
The stability against fragmentation and possible relaxation of the lowest excited states of the Na5F4 cluster (representative of cubic non stoechiometric clusters with an excess sodium atom, also called sodium-tail) is investigated
by means of one-electron pseudopotential calculations with particular reference to photoabsorption processes from the ground
state. Whereas the equilibrium configuration of the ground state has C3v symmetry, the doubly degenerate 12E excited state is affected by a conical intersection and a Jahn-Teller effect associated with the rotation of the sodium
tail around the C3-axis. This yields a “Mexican hat" topology for the lowest sheet with three equivalent Cs minima. Alternatively the 22A1 state has a minimum retaining the C3v symmetry. The dissociation paths of the cluster along the C3-axis into respectively Na4F4 + Na and Na4F3 + NaF are also investigated. Among the former paths, the excited states are found adiabatically stable with respect to the
products. However in the A1 symmetry, fragmentation into NaF exhibits an interesting avoided crossing between configurations correlated respectively
with Na4F3
+ + NaF- and Na4F3 + NaF. Such interaction, similar to the well-known charge exchange processes in elementary molecules might induce non adiabatic
predissociation of the 22A1 state. This mechanism is invoked to explain the differences between R2PI and depletion spectra, correlated with the dissociation
or relaxation of the excited states.
Received 24 March 2000 and Received in final form 11 July 2000 相似文献
4.
A new and general approach is proposed to analyze the dynamics of a colloidal particle interacting with a nearby wall. This
analysis can be used to determine the acting forces even when the system is non-stationary. As an illustration, we use total
internal reflection microscopy to investigate the forces acting on a polystyrene sulfate latex particle as it is receding
from a charged glass surface.
Received 10 October 2002 Published online: 16 April 2003
RID="a"
ID="a"Present address: Department of Polymer Physics, BASF Aktiengesellschaft, 67056 Ludwigshafen, Germany
RID="b"
ID="b"Present address: Arryx. Inc., Chicago, IL 60601, USA 相似文献
5.
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
6.
M. Lontano D. Ryutov 《The European Physical Journal D - Atomic, Molecular, Optical and Plasma Physics》2002,18(3):347-351
We demonstrate the in situ detection of cold 87Rb atoms near a dielectric surface using the absorption of a weak, resonant evanescent wave. We have used this technique in
time of flight experiments determining the density of atoms falling on the surface. A quantitative understanding of the measured
curve was obtained using a detailed calculation of the evanescent intensity distribution. We have also used it to detect atoms
trapped near the surface in a standing-wave optical dipole potential. This trap was loaded by inelastic bouncing on a strong,
repulsive evanescent potential. We estimate that we trap 1.5×104 atoms at a density 100 times higher than the falling atoms.
Received 14 May 2002 Published online 8 October 2002
RID="a"
ID="a"e-mail: spreeuw@science.uva.nl 相似文献
7.
V.V. Klimov M. Ducloy V.S. Letokhov 《The European Physical Journal D - Atomic, Molecular, Optical and Plasma Physics》2002,20(1):133-148
The frequency shift and linewidth variation of an atomic oscillator placed next to a prolate dielectric or metal spheroid
are found within the framework of the classical approach. Both the frequency shift and linewidth are shown to be substantially
dependent on the location of the atom and the form of the nanospheroid and capable of reaching very high values near the surface
of the nanospheroid under plasmon (polariton) resonance conditions. The predictions are compared with those found for spherical
and cylindrical geometries. The prolate spheroid is treated as a model of a needle tip in apertureless optical scanning microscopy.
Effects of sharpness of interaction between the nanospheroid tip and atoms are considered.
Received 2 January 2002 and Received in final form 3 April 2002 Published online 28 June 2002 相似文献
8.
E. Buixaderas V. Porokhonskyy A. Paskhin M. Savinov J. Petzelt 《The European Physical Journal B - Condensed Matter and Complex Systems》2002,30(3):319-329
Barium sodium niobate (BNN) single crystals are studied by IR spectroscopy, time-domain THz transmission spectroscopy, HF
coaxial wave-guide technique and LF dielectric spectroscopy to cover the frequency range 102-1014 Hz in a wide temperature interval. The dielectric response parallel and perpendicular to the polar c-axis is discussed. The ferroelectric transition at T
c
= 830 K is driven by a relaxational soft mode coupled with another central-mode type relaxation which both gradually disappear
on cooling in the ferroelectric phase. Below T
i
the parameters of the expected IR active amplitudon were estimated. The low-temperature permittivity increase on cooling
for the
field direction has been explained by an incipient proper ferroelectric-ferroelastic transition driven by an IR and Raman
active B2-symmetry soft mode.
Received 24 August 2002 Published online 19 December 2002
RID="a"
ID="a"e-mail: buixader@fzu.cz 相似文献
9.
Q. Sun Q. Wang X.G. Gong V. Kumar Y. Kawazoe 《The European Physical Journal D - Atomic, Molecular, Optical and Plasma Physics》2002,18(1):77-81
We report results of the atomic and electronic structures of Al7C cluster using ab initio molecular dynamics with ultrasoft pseudopotentials and generalized gradient approximation. The lowest energy structure is
found to be the one in which carbon atom occupies an interstitial position in Al7 cluster. The electronic structure shows that the recent observation [Chem. Phys. Lett. 316, 31 (2000)] of magic behavior of Al7C- cluster is due to a large highest occupied and lowest unoccupied molecular orbital (HOMO-LUMO) gap which makes Al7C- chemically inert. These results have further led us to the finding of a new neutral magic cluster Al7N which has the same number of valence electrons as in Al7C- and a large HOMO-LUMO gap of 1.99 eV. Further, calculations have been carried out on (Al7N)2 to study interaction between magic clusters.
Received 28 July 2001 相似文献
10.
M. Talanana M. Benakki F. Amalou S. Bouarab C. Demangeat 《The European Physical Journal B - Condensed Matter and Complex Systems》2001,22(4):497-503
We present an ab initio study of the magnetic surface reconstructions of the B2 FeV alloy using a self-consistent tight-binding linearized muffin
tin orbital method developed in the atomic spheres approximation. For (001) and (111), the surface reconstruction stabilizes
configurations unstable in the bulk alloy. When Fe is at the (001) surface, a c(2×2) in-plane antiferromagnetic order is found to be the ground state with magnetic moments of -2.32 and 2.27. A p(1×1) ↓ ferromagnetic order is displayed in case of V toplayer with a magnetic moment of -1.83. At the (111) surface, we obtain for Fe toplayer two solutions p(1×1)↑ and p(2×1). The configuration p(1×1)↑ is found to be the ground state with a magnetic moment per atom of 2.34. For V toplayer, only the p(1×1) ↓ solution is obtained with a moment of -0.84. In all cases, the Fe-V coupling is always antiparallel like in the bulk. Our results are discussed and compared to experiments.
Received 11 August 2000 and Received in final form 8 June 2001 相似文献
11.
Kellerbauer A. Blaum K. Bollen G. Herfurth F. Kluge H.-J. Kuckein M. Sauvan E. Scheidenberger C. Schweikhard L. 《The European Physical Journal D - Atomic, Molecular, Optical and Plasma Physics》2003,22(1):53-64
For a detailed study of the accuracy of the Penning trap mass spectrometer ISOLTRAP all expected sources of uncertainty were
investigated with respect to their contributions to the uncertainty of the final result. In the course of these investigations,
cross-reference measurements with singly charged carbon clusters 12C+
n were carried out. The carbon cluster ions were produced by use of laser-induced desorption, fragmentation, and ionization
of C60 fullerenes and injected into and stored in the Penning trap system. The comparison of the cyclotron frequencies of different
carbon clusters has provided detailed insight into the residual systematic uncertainty of ISOLTRAP and yielded a value of
8×10-9. This also represents the current limit of mass accuracy of the apparatus. Since the unified atomic mass unit is defined
as 1/12 of the mass of the 12C atom, it will be possible to carry out absolute mass measurements with ISOLTRAP in the future.
Received 7 June 2002 Published online 6 November 2002
RID="a"
ID="a"e-mail: a.kellerbauer@cern.ch
RID="b"
ID="b"Current address: Centre de Physique des Particules de Marseille, 13288 Marseille Cedex 9, France. 相似文献
12.
F. Arias de Saavedra E. Buendıa F.J. Gálvez A. Sarsa 《The European Physical Journal D - Atomic, Molecular, Optical and Plasma Physics》2001,13(2):201-206
A generalized Hylleraas-type basis set with three nonlinear parameters is proposed to study three-body systems interacting
via coulomb forces within the framework of non-relativistic quantum mechanics. This basis set improves the rate of convergence
with respect to previous ones, specially for non-symmetric systems and excited states of two electron atoms. Accurate binding
energies and other properties for S-states of helium-like ions, muonic molecules and the positronium negative ion are reported.
Received 21 July 2000 and Received in final form 4 October 2000 相似文献
13.
Ngai KL 《The European physical journal. E, Soft matter》2002,8(2):225-235
Large increases of mobility of local segmental relaxation observed in polymer films as the film thickness is decreased, as
evidenced by decreases of the glass temperature, are not found for relaxation mechanisms that have longer length scales including
the Rouse relaxation modes and the diffusion of entire polymer chains. We show that the coupling model predictions, when extended
to consider polymer thin films, are consistent with a large increase of the mobility of the local segmental motions and the
lack of such a change for the Rouse modes and the diffusion of entire polymer chains. There are two effects that can reduce
the coupling parameter of the local segmental relaxation in thin films. One is the chain orientation that is induced parallel
to the surface when the film thickness h becomes smaller than the end-to-end distance of the chains and the other is a finite-size effect when h is no longer large compared to the cooperative length scale. Extremely thin ( ≈ 1.5 nm) films obtained by intercalating a
polymer into layered silicates have thickness significantly less than the cooperative length scale near the bulk polymer glass
transition temperature. As a result, the coupling parameter of the local segmental relaxation in such thin films is reduced
almost to zero. With this plausible assumption, we show the coupling model can explain quantitatively the large decrease of
the local segmental relaxation time found experimentally.
Received 1 August 2001 and Received in final form 1 December 2001 相似文献
14.
P. Mélinon F. Tournus B. Masenelli A. Perez M. Pellarin J. Lermé M. Broyer B. Champagnon 《The European Physical Journal D - Atomic, Molecular, Optical and Plasma Physics》2001,16(1):337-340
This paper deals with a new type of SiC bonding where silicon atom seems to bridge C60 molecules. We have studied films obtained by deposition of (C60)nSim clusters prepared in a laser vaporization source. Prior deposition, free ionized clusters were studied in a time-of-flight
mass spectrometer. Mixed clusters (C60)nSim were clearly observed. Abundance and photofragmentation mass spectroscopies revealed the relatively high stability of the
(C60)nSi
n
+
, (C60)nSi
n - 1
+
and (C60)nSi
n - 2
+
species. This observation is in favor of the arrangement of these complexes as polymers where the C60 cages may be bridged by a silicon atom. Free neutral clusters are then deposited onto substrate making up a nanogranular
thin film (≃ 100 nm). The film is probed by Auger and X-ray photoemission spectroscopies, but above all by surface enhanced Raman scattering.
The results suggest an unusual chemical bonding between silicon and carbon and the environment of the silicon atom is expected
to be totally different from the sp3 lattice: ten or twelve carbon neighbors might surround silicon atom. The bonding is discussed to the light of the so-called
fullerene polymerization as observed for pure fullerite upon laser irradiation. This opens a new route for bridging C60 molecules together with an appreciable energy bonding, since the usual van der Waals bonding in fullerite could be replaced
by an ionocovalent bond. Such an assumption must be checked in the future by XAS and EXAFS experiments.
Received 15 November 2000 相似文献
15.
Z. Iqbal Y. Zhang H. Grebel S. Vijayalakshmi A. Lahamer G. Benedek M. Bernasconi J. Cariboni I. Spagnolatti R. Sharma F.J. Owens M.E. Kozlov K.V. Rao M. Muhammed 《The European Physical Journal B - Condensed Matter and Complex Systems》2003,31(4):509-515
Evidence is presented for the formation of a solid phase based on the smallest fullerene, C20, in thin diamond-like carbon films deposited by ultraviolet laser ablation from diamond onto nickel substrates at room temperature
in the presence of 10-4 torr of cyclohexane or benzene. Laser desorption mass spectrometry from the films shows the presence of C20, C21 and C22 species, while micro-Raman spectroscopy and electron diffraction from selected particles together with first principle density-functional
calculations, indicate a cubic solid with dodecahedral C20 cages as building blocks. Unlike solid C60 and fully protonated C20, which are bound by van der Waals forces, the proposed structure is stabilized by linking of the C20 dodecahedra with bridging carbon atoms at interstitial tetrahedral sites to form a face-centered-cubic lattice with 22 carbon
atoms per unit cell.
Received 10 October 2002 / Received in final form 24 December 2002 Published online 6 March 2003
RID="a"
ID="a"e-mail: zafar.iqbal@njit.edu 相似文献
16.
Linear stability analysis of capillary instabilities in a thin nematic liquid crystalline cylindrical fiber embedded in an
immiscible viscous matrix is performed by formulating and solving the governing nemato-capillary equations, that include the
effect of temperature on the nematic ordering as well as the effect of the nematic orientation. A representative axial nematic
orientation texture with the planar easy axis at the fiber surface is studied. The surface disturbance is expressed in normal
modes, which include the azimuthal wave number m to take into account non-axisymmetric modes. Capillary instabilities in nematic fibers reflect the anisotropic nature of
liquid crystals, such as the ordering and orientation contributions to the surface elasticity and surface normal and bending
stresses. Surface gradients of normal and bending stresses provide additional anisotropic contributions to the capillary pressure
that may renormalize the classical displacement and curvature forces that exist in any fluid fiber. The exact nature (stabilizing
and destabilizing) and magnitude of the renormalization of the displacement and curvature forces depend on the nematic ordering
and orientation, i.e. the anisotropic contribution to the surface energy, and accordingly capillary instabilities may be axisymmetric or non-axisymmetric.
In addition, when the interface curvature effects are accounted for as contributions of the work of interfacial bending and
torsion to the total energy of the system, the higher-order bending moment contribution to the surface stress tensor is critical
in stabilizing the fiber instabilities. For the planar easy axis, the nematic ordering contribution to the surface energy,
which renormalizes the effect of the fiber shape, plays a crucial role to determine the instability mechanisms. Moreover,
the unstable modes, which are most likely observed, can be driven by the dependence of surface energy on the surface area.
Low-ordering fibers display the classical axisymmetric mode, since the surface energy decreases by decreasing the surface
area. Decreasing temperature gives rise to the encounter with a local maximum or to monotonic increase of the characteristic
length of the axisymmetric mode. Meanwhile, in the presence of high surface ordering, non-axisymmetric finite wavelength instabilities
emerge, with higher modes growing faster since the surface energy decreases by increasing the surface area. As temperature
decreases, the pitches of the chiral microstructures become smaller. However, this non-axisymmetric instability mechanism
can be regulated by taking account of the surface bending moment, which contains higher order variations in the interface
curvatures. More and more non-axisymmetric modes emerge as temperature decreases, but, at constant temperature, only a finite
number of non-axisymmetric modes are unstable and a single fastest growing mode emerges with lower and higher unstable modes
growing slower. For nematic fibers, the classical fiber-to-droplet transformation is one of several possible instability pathways,
while others include chiral microstructures. The capillary instabilities' growth rate of a thin nematic fiber in a viscous
matrix is suppressed by increasing either the fiber or matrix viscosity, but the estimated droplet sizes after fiber breakup
in axisymmetric instabilities decrease with increasing the matrix viscosity.
Received 15 April 2002 and Received in final form 3 October 2002
RID="a"
ID="a"e-mail: alejandro.rey@mcgill.ca 相似文献
17.
Using Monte Carlo simulations, we study the counterion distribution close to planar charged walls in two geometries: i) when
only one charged wall is present and the counterions are confined to one half-space, and ii) when the counterions are confined
between two equally charged walls. In both cases the surface charge is smeared out and the dielectric constant is the same
everywhere. We obtain the counterion density profile and compare it with both the Poisson-Boltzmann theory (asymptotically
exact in the limit of weak coupling, i.e. low surface charge, high temperature and low counterion valence) and the strong-coupling theory (valid in the opposite limit
of high surface charge, low temperature and high counterion valence) and with previously calculated correction terms to both
theories for different values of the coupling parameter, thereby establishing the domain of validity of the asymptotic limits.
Gaussian corrections to the leading Poisson-Boltzmann behavior (obtained via a systematic loop expansion) in general perform quite poorly: At coupling strengths low enough so that the Gaussian (or one-loop)
correction does describe the numerical deviations from the Poisson-Boltzmann result correctly, the leading Poisson-Boltzmann
term by itself matches the data within high accuracy. This reflects the slow convergence of the loop expansion. For a single
charged plane, the counterion pair correlation function indicates a behavioral change from a three-dimensional, weakly correlated
counterion distribution (at low coupling) to a two-dimensional, strongly correlated counterion distribution (at high coupling),
which is paralleled by the specific-heat capacity which displays a rounded hump at intermediate coupling strengths. For the
case of counterions confined between two equally charged walls, we analyze the inter-wall pressure and establish the complete
phase diagram, featuring attraction between the walls for large enough coupling strength and at intermediate wall separation.
Depending on the thermodynamic ensemble, the phase diagram exhibits a discontinuous transition where the inter-wall distance
jumps to infinity (in the absence of a chemical potential coupling to the inter-wall distance, as for charged lamellae in
excess solvent) or a critical point where two coexisting states with different inter-wall distance become indistinguishable
(in the presence of a chemical potential, as for charged lamellae with a finite fixed solvent fraction). The attractive pressure
decays with the inter-wall distance as an inverse cube, similar to analytic predictions, although the amplitude differs by
an order of magnitude from previous theoretical results. Finally, we discuss in detail our simulation methods and compare
the finite-size scaling behavior of different boundary conditions (periodic, minimal image and open).
Received 6 November 2001 相似文献
18.
E. Jahier J. Guéna Ph. Jacquier M. Lintz M.A. Bouchiat 《The European Physical Journal D - Atomic, Molecular, Optical and Plasma Physics》2001,17(2):221-229
We demonstrate the production of an electric field inside a high temperature cesium vapor cell with external electrodes. This external control of the electric field, which is not possible with a glass cell in presence of a cesium
vapor, is achieved using a cell made of sapphire, and is of particular interest for our ongoing Parity Violation experiment.
We describe the main components and the implementation on the set-up, including the pulsed high voltage generator. With pulse
duration not exceeding 200 ns the system provides a reversible longitudinal E-field of up to 2 kV/cm in the vapor at a density of ∼ 2×1014 at/cm3 without discharge. Atomic signals attest the application of the electric field in the cell, with the predicted value. Further
improvements obtained with sapphire cells are also presented.
Received 15 September 2000 相似文献
19.
Engineering entanglement of a general three-level system interacting with a correlated two-mode nonlinear coherent state 总被引:2,自引:0,他引:2
Mahmoud Abdel-Aty Abdel-Shafy F. Obada 《The European Physical Journal D - Atomic, Molecular, Optical and Plasma Physics》2003,23(1):155-165
In this article a treatment of a three-level atom interacting with two modes of light in a cavity with arbitrary forms of
nonlinearities of both the fields and the intensity-dependent atom-field coupling is presented. A factorization of the initial
density operator is assumed, with the privileged field modes being in a pair-coherent state. We derive and illustrate an exact
expression for the time evolution of the density operator, by means of which we identify and numerically demonstrate the region
of parameters where significantly large entanglement can be obtained. We show that entanglement can be significantly influenced
by different kinds of nonlinearities. The nonlinear medium yields the superstructure of atomic Rabi oscillation. We propose
a generation of Bell-type states having a simple initial state preparation of the present system.
Received 29 July 2002 / Received in final form 18 October 2002 Published online 21 January 2003
RID="a"
ID="a"e-mail: abdelaty@uni-flensburg.dePresent address: Institut für Mathematik, Universit?t Flensburg, Germany. 相似文献
20.
X. Wu A.K. Ray 《The European Physical Journal B - Condensed Matter and Complex Systems》2001,19(3):345-351
The electronic and geometric structures of bulk PuO2 and its (110) surface have been studied using a periodic model within the generalized gradient approximation (GGA) of density
functional theory (DFT). The sixty core electrons of the Pu atom have been represented by a relativistic effective core potential
and scalar relativistic effects have been incorporated on the valence orbitals. For bulk PuO2, we predict an equilibrium lattice constant of 10.10 a.u. and a cohesive energy of 17.28 eV, in good agreement with experimental
data. For the (110) surface, upon relaxation, the distance between the top layer and the next layer is found to decrease by
0.12 ?, i.e. 5.3% of the corresponding interlayer distance in the bulk. The distance between the two oxygen atoms on the top layer is
found to increase by 0.15 ?, i.e. 5.6% of the corresponding bulk value. The small surface relaxation energy of 0.268 eV per unit cell indicates the fair stability
of this surface. The effective charges on Pu and O atoms show that the chemical bonding in this system is not purely ionic.
Together with the metallic feature of the density of states (DOS) on the surface, the effective charge distribution provides
some basis for understanding surface reactivity and corresponding support for catalysis.
Received 16 June 2000 相似文献