18,296 research outputs found
On the premelting features in sodium clusters
Melting in Na_n clusters described with an empirical embedded-atom potential
has been reexamined in the size range 55<=n<=147 with a special attention at
sizes close to 130. Contrary to previous findings, premelting effects are also
present at such medium sizes, and they turn out to be even stronger than the
melting process itself for Na_133 or Na_135. These results indicate that the
empirical potential is_qualitatively_ unadequate to model sodium clusters.Comment: 4 pages, 3 postscript figure
Theoretical study of the finite temperature spectroscopy in van der Waals clusters. III Solvated Chromophore as an effective diatomics
The absorption spectroscopy of calcium-doped argon clusters is described in
terms of an effective diatomics molecule Ca-(Ar_n), in the framework of
semiclassical vertical transitions. We show how, upon choosing a suitable
reaction coordinate, the effective finite-temperature equilibrium properties
can be obtained for the ground- and excited-surfaces from the potential of mean
force (PMF). An extension of the recent multiple range random-walk method is
used to calculate the PMF over continuous intervals of distances. The
absorption spectra calculated using this single-coordinate description are
found to be in good agreement with the spectra obtained from high-statistics
Monte Carlo data, in various situations. For CaAr, we compare the
performances of two different choices of the reaction coordinate. For CaAr_37,
the method is seen to be accurate enough to distinguish between different
low-energy structures. Finally, the idea of casting the initial many-body
problem into a single degree of freedom problem is tested on the spectroscopy
of calcium in bulk solid argon.Comment: 8 pages, 9 figure
Statistical evaporation of rotating clusters. II. Angular momentum distribution
The change in the angular momentum of an atomic cluster following evaporation
is investigated using rigorous phase space theory and molecular dynamics
simulations, with an aim at the possible rotational cooling and heating
effects. Influences of the shape of the interaction potential, anharmonicity of
the vibrational density of states (DOS), and the initial distribution of
excitation energies are systematically studied on the example of the
Lennard-Jones cluster LJ_14. For this system, the predictions of PST are in
quantitative agreement with the results of the simulations, provided that the
correct forms for the vibrational density of states and the interaction
potential are used. The harmonic approximation to the DOS is used to obtain
explicit forms for the angular momentum distribution in larger clusters. These
are seen to undergo preferential cooling when thermally excited, and
preferential heating when subject to a strong vibrational excitation.Comment: 10 pages, 7 figure
Theoretical study of finite temperature spectroscopy in van der Waals clusters. II Time-dependent absorption spectra
Using approximate partition functions and a master equation approach, we
investigate the statistical relaxation toward equilibrium in selected CaAr
clusters. The Gaussian theory of absorption (previous article) is employed to
calculate the average photoabsorption intensity associated with the 4s^2->
4s^14p^1 transition of calcium as a function of time during relaxation. In
CaAr_6 and CaAr_10 simple relaxation is observed with a single time scale.
CaAr_13 exhibits much slower dynamics and the relaxation occurs over two
distinct time scales. CaAr_37 shows much slower relaxation with multiple
transients, reminiscent of glassy behavior due to competition between different
low-energy structures. We interpret these results in terms of the underlying
potential energy surfaces for these clusters.Comment: 10 pages, 9 figure
Kinetic approach to the cluster liquid-gas transition
The liquid-gas transition in free atomic clusters is investigated
theoretically based on simple unimolecular rate theories and assuming
sequential evaporations. A kinetic Monte Carlo scheme is used to compute the
time-dependent properties of clusters undergoing multiple dissociations, and
two possible definitions of the boiling point are proposed, relying on the
cluster or gas temperature. This numerical approach is supported by molecular
dynamics simulations of clusters made of sodium atoms or C60 molecules, as well
as simplified rate equation
Antiferromagnetic spin chain behavior and a transition to 3D magnetic order in Cu(D,L-alanine)2: Roles of H-bonds
We study the spin chain behavior, a transition to 3D magnetic order and the
magnitudes of the exchange interactions for the metal-amino acid complex
Cu(D,L-alanine)2.H2O, a model compound to investigate exchange couplings
supported by chemical paths characteristic of biomolecules. Thermal and
magnetic data were obtained as a function of temperature (T) and magnetic field
(B0). The magnetic contribution to the specific heat, measured between 0.48 and
30 K, displays above 1.8 K a 1D spin-chain behavior that can be fitted with an
intrachain antiferromagnetic (AFM) exchange coupling constant 2J0 = (-2.12
0.08) cm, between neighbor coppers at 4.49 {\AA} along chains
connected by non-covalent and H-bonds. We also observe a narrow specific heat
peak at 0.89 K indicating a phase transition to a 3D magnetically ordered
phase. Magnetization curves at fixed T = 2, 4 and 7 K with B0 between 0 and 9
T, and at T between 2 and 300 K with several fixed values of B0 were globally
fitted by an intrachain AFM exchange coupling constant 2J0 = (-2.27 0.02)
cm and g = 2.091 0.005. Interchain interactions J1 between coppers
in neighbor chains connected through long chemical paths with total length of
9.51 {\AA} are estimated within the range 0.1 < |2J1| < 0.4 cm, covering
the predictions of various approximations. We analyze the magnitudes of 2J0 and
2J1 in terms of the structure of the corresponding chemical paths. The main
contribution in supporting the intrachain interaction is assigned to H-bonds
while the interchain interactions are supported by paths containing H-bonds and
carboxylate bridges, with the role of the H-bonds being predominant. We compare
the obtained intrachain coupling with studies of compounds showing similar
behavior and discuss the validity of the approximations allowing to calculate
the interchain interactions.Comment: 10 pages, 4 figure
Sampling along reaction coordinates with the Wang-Landau method
The multiple range random walk algorithm recently proposed by Wang and Landau
[Phys. Rev. Lett. 86, 2050 (2001)] is adapted to the computation of free energy
profiles for molecular systems along reaction coordinates. More generally, we
show how to extract partial averages in various statistical ensembles without
invoking simulations with constraints, biasing potentials or unknown
parameters. The method is illustrated on a model 10-dimensional potential
energy surface, for which analytical results are obtained. It is then applied
to the potential of mean force associated with the dihedral angle of the butane
molecule in gas phase and in carbon tetrachloride solvent. Finally,
isomerization in a small rocksalt cluster, Na4F4, is investigated in the
microcanonical ensemble, and the results are compared to those of parallel
tempering Monte Carlo.Comment: 6 pages, 5 figure
Spin-induced angular momentum switching
When light is transmitted through optically inhomogeneous and anisotropic
media the spatial distribution of light can be modified according to its input
polarization state. A complete analysis of this process, based on the paraxial
approximation, is presented, and we show how it can be exploited to produce a
spin-controlled-change in the orbital angular momentum of light beams
propagating in patterned space-variant-optical-axis phase plates. We also
unveil a new effect. The development of a strong modulation in the angular
momentum change upon variation of the optical path through the phase plates.Comment: The original paper of the published version in Opt. Let
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