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char = s;code = 115
char = :;code = 58
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char = ;code = 32
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char = k;code = 107
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char = g;code = 103
char = e;code = 101
char = ?;code = 63
result sql = Solid-solution precursor to melting in onion-ring Pd-Pt nanoclusters: a case of second-order-like phase change?
Solid-solution precursor to melting in onion-ring Pd-Pt nanoclusters: a case of second-order-like phase change?
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result sql = The thermodynamical behaviour of icosahedral, multilayer Pd-Pt clusters is addressed using a combination of simulation tools, mainly parallel tempering Monte Carlo. A preferential swapping trial move is introduced to increase the chance of successfully exchanging Pd and Pt atoms in the cluster. The 2-, 3- and 4-shell, Pd-rich clusters have been studied. We generally find that the clusters melt at a temperature significantly below the bulk melting point at the same corresponding composition. More interestingly, for the smaller clusters melting is initiated by a solid-solution intermediate phase in which the overall icosahedral frame remains, but the Pd and Pt atoms can swap sites. The transition to this solid-solution phase is seen to have a continuous, second-order like character, which is interpreted from the similarity between the present system with the ferromagnetic Ising model on the 3D cubic lattice. As the cluster grows, the onion-ring structure becomes thermodynamically unstable. The 4-layer cluster already exhibits a solid-solution in its core at temperatures as low as 100 K. The bulk behaviour is thus recovered at very small scales.

Publication: Faraday Discuss. 2008 ;138:75-88; discussion 119-35, 433-4.
Publication Date: 2008
Study Author(s): Calvo, Florent;
Institution: LASIM, Université Claude Bernard Lyon I, Lyon, France. [email protected]
Shortcut link to this study:
The thermodynamical behaviour of icosahedral, multilayer Pd-Pt clusters is addressed using a combination of simulation tools, mainly parallel tempering Monte Carlo. A preferential swapping trial move is introduced to increase the chance of successfully exchanging Pd and Pt atoms in the cluster. The 2-, 3- and 4-shell, Pd-rich clusters have been studied. We generally find that the clusters melt at a temperature significantly below the bulk melting point at the same corresponding composition. More interestingly, for the smaller clusters melting is initiated by a solid-solution intermediate phase in which the overall icosahedral frame remains, but the Pd and Pt atoms can swap sites. The transition to this solid-solution phase is seen to have a continuous, second-order like character, which is interpreted from the similarity between the present system with the ferromagnetic Ising model on the 3D cubic lattice. As the cluster grows, the onion-ring structure becomes thermodynamically unstable. The 4-layer cluster already exhibits a solid-solution in its core at temperatures as low as 100 K. The bulk behaviour is thus recovered at very small scales.
PMID: 18447010

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