McClurg, Richard B. and Flagan, Richard C. and Goddard, Willam A., III (1995) Free energy and surface tension of arbitrarily large Mackay icosahedral clusters. Journal of Chemical Physics, 102 (8). pp. 3322-3330. ISSN 0021-9606. http://resolver.caltech.edu/CaltechAUTHORS:MCCjcp95
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We present a model for predicting the free energy of arbitrarily large Mackay icosahedral clusters. van der Waals clusters are experimentally observed to be particularly stable at magic numbers corresponding to these structures. Explicit calculations on the vibrational states were used to determine the spectrum of fundamental frequencies for smaller (<=561) icosahedral clusters. The scaled cumulative frequency distribution function rapidly approaches a limiting function for large clusters. This function was used to predict zero-point energies and vibrational free energies for larger clusters (>~561 atoms). Combining these predictions with correlations for the moment of inertia and for the minimum potential energy of large clusters leads to free energies of arbitrary large clusters. The free energies are used to predict the chemical potential and surface tension as a function of size and temperature. This connects macroscopic properties to the microscopic atomic parameters.
|Additional Information:||©1995 American Institute of Physics. (Received 26 August 1994; accepted 11 November 1994) We thank Dr. Guanhua Chen for helpful discussions, Dr. Terry Coley for assistance with the vibrational calculations on large systems, and Dr. Siddharth Dasgupta for modifications to POLYGRAF. R.B M. acknowledges a National Science Foundation Graduate Research Fellowship. Partial support of the work was provided by grants from the NSF (Nos. CHE 91-100289, CTS 91-13191, and ASC 9217368). The computer facilities of the MSC used in this work are also supported by grants from DOE-AICD, Allied-Signal Corp., Asahi Chemical, Asahi Glass, BP America, Chevron, BF Goodrich, Teijin Ltd., Vestar, Hughes Research Laboratories, Xerox, and Beckman Institute.|
|Subject Keywords:||FREE ENERGY; SURFACE TENSION; VAN DER WAALS FORCES; VIBRATIONAL STATES; DISTRIBUTION FUNCTIONS; ZERO–POINT ENERGY; ATOMIC CLUSTERS; MOMENT OF INERTIA; POTENTIAL ENERGY; CHEMICAL POTENTIAL; SIZE; TEMPERATURE DEPENDENCE|
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|Deposited On:||24 Dec 2005|
|Last Modified:||26 Dec 2012 08:43|
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