Melting and freezing in isothermal Ar13 clusters

Davis, Heidi L.; Jellinek, Julius; Berry, R. Stephen

doi:10.1063/1.452436

Cited by 203 publications

(107 citation statements)

References 18 publications

Supporting

Mentioning

104

Contrasting

Order By: Relevance

“…(1) by employing Feynman path integrals' p (x,x';P> = s Dx(u)expC-S[x(u>lI, (2) We begin in Sec. II with a brief review of the FPI method and the essential concepts that pertain to J walking.…”

Section: Action Integralsmentioning

confidence: 99%

Extending J walking to quantum systems: Applications to atomic clusters

Frantz

Freeman

Doll

1992

The Journal of Chemical Physics

View full text Add to dashboard Cite

The J-walking (or jump-walking) method is extended to quantum systems by incorporating it into the Fourier path integral Monte Carlo methodology. J walking can greatly reduce systematic errors due to quasiergodicity, or the incomplete sampling of configuration space in Monte Carlo simulations. As in the classical case, quantum J walking uses a jumping scheme ,to overcome configurational barriers. It couples the usual Metropolis sampling to a distribution generated at a higher temperature where the sampling is sufficiently ergodic. The J-walker distributions used in quantum J walking can be either quantum or classical, with classical distributions having the advantage of lower storage requirements, but the disadvantage of being slightly more computationally intensive and having a more limited useful temperature range. The basic techniques are illustrated first on a simple onedimensional double well potential based on a quartic polynomial. The suitability of J walking for typical multidimensional quantum Monte Carlo systems is then shown by applying the method to a multiparticle cluster system consisting of rare gas atoms bound by pairwise Lennard-Jones potentials. Different degrees of quantum behavior are considered by examining both argon and neon clusters. Remarkable improvements in the convergence rate for the cluster energy and heat capacity, analogous to those found in classical systems, are found for temperatures near the cluster transition regions.

show abstract

Section: Action Integralsmentioning

confidence: 99%

Extending J walking to quantum systems: Applications to atomic clusters

Frantz

Freeman

Doll

1992

The Journal of Chemical Physics

View full text Add to dashboard Cite

show abstract

“…This is confirmed by the distribution on the total kinetic energy of cluster atoms [3] under adiabatic conditions that has a bimodal form (Fig. 3), so that the cluster is This determines the character of phase coexistence that relates to conditions of a microcanonical [3] and canonical [19] atom ensemble. Such a form of phase coexistence together with relatively large times of location in each aggregate state allows one to consider a cluster as a thermodynamic object.…”

Section: Phase Transition In 13-atom Clustermentioning

confidence: 60%

“…The entropy jump at melting of the isothermal 13-atom Lennard-Jones cluster. Closed circles are obtained from the results of computer simulation of the isolated 13-atom Lennard-Jones cluster [3], and close circles relate to the isothermal 13-atom Lennard-Jones cluster [19]. Projections of PES on a sphere in a many-dimensional coordinate space for a 13-atom cluster of an inert gas (a) and for a 13-atom metal cluster (b).…”

Section: Phase Transition In 13-atom Clustermentioning

confidence: 99%

“…One can determine the total entropy jump on the basis of dynamic cluster simulations using formula (6). This operation was done on the basis cluster simulations where the 13-atom Lennard-Jones was a microcanonical [3] and canonical [19] ensemble of atoms. The results are reduced to the canonical case and are given in Fig.…”

Section: Phase Transition In 13-atom Clustermentioning

confidence: 99%

See 1 more Smart Citation

Phase transitions in clusters

Berry

Smirnov

2009

Low Temperature Physics

View full text Add to dashboard Cite

General concepts of cluster phase transitions are reviewed as well as the cluster behavior near the melting point. Configuration excitation determines the nature of the cluster phase transitions, but a significant contribution to the entropy jump is given by thermal motion of atoms that allows one to characterize the phase transition through thermal atom motion in the Lindemann and other criteria. The phase coexistence near the melting point is the peculiarity of not large clusters. The void concept of phase transitions with a void as an elementary configuration excitation allows one to describe the phase transition for clusters and macroscopic atomic systems. Phase transitions in metal clusters resemble those in clusters with pairwise atomic interactions, but their numerical parameters are other because of a large number of isomers and an additional electron degree of freedom. Cluster models are convenient for the analysis of macroscopic atomic systems. They allow us to understand the nature of glassy transitions and the reason of absence of a stable infinite crystal lattice for gases at zero temperature and high pressure.

show abstract

“…Cluster thermodynamics have been studied using molecular dynamics ͑MD͒ 3,12,[16][17][18][19] and Monte Carlo ͑MC͒ 12,[19][20][21][22][23][24] simulations, and statistical-mechanical modeling. 12,18 All three approaches face a formidable challenge: sampling of the potential surface in sufficient detail to faithfully represent the thermodynamically accessible regions.…”

Section: Introductionmentioning

confidence: 99%

Thermodynamic properties and homogeneous nucleation rates for surface-melted physical clusters

McClurg

Flagan

Goddard

1996

The Journal of Chemical Physics

View full text Add to dashboard Cite

We predict the free energy of van der Waals clusters (F n ) in the surface-melted temperature regime. These free energies are used to predict the bulk chemical potential, surface tension, Tolman length, and vapor pressure of noble gas crystals. Together, these estimates allow us to make definitive tests of the capillarity approximation in classical homogeneous nucleation theory. We find that the capillarity approximation underestimates the nucleation rate by thirty orders of magnitude for argon. The best available experiments are consistent with our calculation of nucleation rate as a function of temperature and pressure. We suggest experimental conditions appropriate for determining quantitative nucleation rates which would be invaluable in guiding further development of the theory. To make the predictions of F n , we develop the Shellwise Lattice Search ͑SLS͒ algorithm to identify isomer fragments and the Linear Group Contribution ͑LGC͒ method to estimate the energy of isomers composed of those fragments. Together, SLS/LGC approximates the distribution of isomers which contribute to the configurational partition function ͑for up to 147-atom clusters͒. Estimates of the remaining free energy contributions come from a previous paper in this series.

show abstract

Melting and freezing in isothermal Ar13 clusters

Cited by 203 publications

References 18 publications

Extending J walking to quantum systems: Applications to atomic clusters

Extending J walking to quantum systems: Applications to atomic clusters

Phase transitions in clusters

Thermodynamic properties and homogeneous nucleation rates for surface-melted physical clusters

Contact Info

Product

Resources

About