Second-Order Phase Transitions in Amorphous Gallium Clusters

Breaux, Gary A.; Cao, Bangwei; Jarrold, Martin F.

doi:10.1021/jp052887x

Cited by 54 publications

(98 citation statements)

References 37 publications

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“…Another possible explanation is that the clusters melt within the temperature range examined here, but that they melt without a latent heat. This behavior has recently been found in experimental stud- ies of small gallium clusters [23]. It has also been observed in molecular dynamics simulations where it has been found to occur for clusters that have disordered ground states.…”

Section: Discussionsupporting

confidence: 64%

“…If these features are due to melting, there is a spectacular jump in the melting temperature between 62 (453 K) and 66 (902 K) atoms. Such a large jump forces us to ask if there could be another explanation for the small maxima in the heat capacities at around 900 K. For example, some gallium clusters have been shown to melt without a significant peak in the heat capacity [23]. Could the cluster melt at a lower temperature and the peaks observed at around 900 K be due to a liquid-to-liquid phase transition?…”

Section: Resultsmentioning

confidence: 99%

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Ion calorimetry: Using mass spectrometry to measure melting points

Neal

Starace

Jarrold

2007

J. Am. Soc. Mass Spectrom.

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Calorimetry measurements have been used to probe the melting of aluminum cluster cations with 63 to 83 atoms. Heat capacities were determined as a function of temperature (from 150 to 1050 K) for size-selected cluster ions using an approach based on multicollision-induced dissociation. The experimental method is described in detail and the assumptions are critically evaluated. Most of the aluminum clusters in the size range examined here show a distinct peak in their heat capacities that is attributed to a melting transition (the peak is due to the latent heat). The melting temperatures are below the bulk melting point and show enormous fluctuations as a function of cluster size. Some clusters (for example, n ϭ 64, 68, and 69) do not show peaks in their heat capacities. This behavior is probably due to the clusters having a disordered solid-like phase, so that melting occurs without a latent heat. (J Am Soc Mass Spectrom 2007, 18, 74 -81)

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Section: Discussionsupporting

confidence: 64%

Section: Resultsmentioning

confidence: 99%

Ion calorimetry: Using mass spectrometry to measure melting points

Neal

Starace

Jarrold

2007

J. Am. Soc. Mass Spectrom.

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“…There is price to pay however because the determination of the amount of energy transferred by inelastic collisions relies on a model. Another method, which is not based on the determination of the caloric curve, has been used to extract melting temperatures [9]: one measures the mobility of clusters in a drift tube, from which collision cross sections are deduced. A variation of the cross section as a function of the temperature is the signature of the phase transition.…”

Section: Introductionmentioning

confidence: 99%

A novel experimental method for the measurement of the caloric curves of clusters

Chirot

Feiden

Zamith

et al. 2008

The Journal of Chemical Physics

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A novel experimental scheme has been developed in order to measure the heat capacity of mass selected clusters. It is based on controlled sticking of atoms on clusters. This allows one to construct the caloric curve, thus determining the melting temperature and the latent heat of fusion in the case of first-order phase transitions. This method is model-free. It is transferable to many systems since the energy is brought to clusters through sticking collisions. As an example, it has been applied to N a

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“…The initial work on cationic clusters of 17, 39, and 40 atoms was followed by a systematic study of the 29-50 atom size range, from which the effects of addition or removal of a single atom became apparent [66]. Notably, single atoms were shown to account for differences of hundreds of Kelvin in the melting temperature, and for variations also in the nature of the melting transition itself, which could be better described as second-order in certain cases, implying the existence of amorphous structures in the solid state.…”

Section: Beyond Melting Point Depressionmentioning

confidence: 99%

Cluster melting: new, limiting, and liminal phenomena

Gaston

2018

Advances in Physics: X

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The thermodynamic behaviour of clusters and nanoscale structures is both a challenge to the statistical basis of the theory, and of paramount importance to experiment. In this review, the competing influences that determine the melting temperature and behaviour of small atomic clusters is discussed, with reference to both experiment and theory. The liminal spaces between solid and liquid, the non-scaling and scaling regimes, and the metallic and non-metallic states are discussed, and presented as a primary cause of the emergence of new phenomena. Particular emphasis is given to recent theoretical work that combines each of these liminal regions and enables, through first principles calculations of dynamic atomic interactions in Born Oppenheimer molecular dynamics, the explanation of greater than bulk melting temperatures in certain atomic cluster systems. Some perspective is also given on the important questions in nanoscale thermodynamics that remain to be addressed. ARTICLE HISTORY

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Second-Order Phase Transitions in Amorphous Gallium Clusters

Cited by 54 publications

References 37 publications

Ion calorimetry: Using mass spectrometry to measure melting points

Ion calorimetry: Using mass spectrometry to measure melting points

A novel experimental method for the measurement of the caloric curves of clusters

Cluster melting: new, limiting, and liminal phenomena

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