Abstract
The internal energy distributions for melting aluminum cluster cations with 100, 101, 126, and 127 atoms have been investigated using multicollision induced dissociation. The experimental results can be best fit with a statistical thermodynamic model that incorporates only fully solidlike and fully liquidlike clusters so that the internal energy distributions become bimodal during melting. This result is consistent with computer simulations of small clusters, where rapid fluctuations between entirely solidlike and entirely liquidlike states occur during the phase change. To establish a bimodal internal energy distribution, the time between the melting and freezing transitions must be longer than the time required for equilibration of the energy distribution (which is estimated to be around 1–2 μs under our conditions). For Al100+ and Al101+, the results indicate that this criterion is largely met. However, for Al126+ and Al127+, it appears that the bimodal energy distributions are partly filled in, suggesting that either the time between the melting and freezing transitions is comparable to the equilibration time or that the system starts to switch to macroscopic behavior where the phase change occurs with the two phases in contact.
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Dates
Type | When |
---|---|
Created | 16 years, 2 months ago (May 26, 2009, 6:26 p.m.) |
Deposited | 2 years, 2 months ago (June 19, 2023, 10:59 p.m.) |
Indexed | 3 weeks, 3 days ago (July 30, 2025, 6:52 a.m.) |
Issued | 16 years, 2 months ago (May 26, 2009) |
Published | 16 years, 2 months ago (May 26, 2009) |
Published Online | 16 years, 2 months ago (May 26, 2009) |
Published Print | 16 years, 2 months ago (May 28, 2009) |
@article{Cao_2009, title={Phase coexistence in melting aluminum clusters}, volume={130}, ISSN={1089-7690}, url={http://dx.doi.org/10.1063/1.3129525}, DOI={10.1063/1.3129525}, number={20}, journal={The Journal of Chemical Physics}, publisher={AIP Publishing}, author={Cao, Baopeng and Starace, Anne K. and Judd, Oscar H. and Jarrold, Martin F.}, year={2009}, month=may }