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Journal of Chemical Physics / Volume 136 / Issue 8 / ARTICLES / Surfaces, Interfaces, and Materials

J. Chem. Phys. 136, 084701 (2012); http://dx.doi.org/10.1063/1.3685835 (8 pages)

Sensitivity of nucleation phenomena on range of interaction potential

Rakesh S. Singh, Mantu Santra, and Biman Bagchi

Solid State and Structural Chemistry Unit, Indian Institute of Science, Bangalore 560012, India

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(Received 18 August 2011; accepted 26 January 2012; published online 22 February 2012)

Theoretical and computational investigations of nucleation have been plagued by the sensitivity of the phase diagram to the range of the interaction potential. As the surface tension depends strongly on the range of interaction potential and as the classical nucleation theory (CNT) predicts the free energy barrier to be directly proportional to the cube of the surface tension, one expects a strong sensitivity of nucleation barrier to the range of the potential; however, CNT leaves many aspects unexplored. We find for gas-liquid nucleation in Lennard-Jones system that on increasing the range of interaction the kinetic spinodal (KS) (where the mechanism of nucleation changes from activated to barrierless) shifts deeper into the metastable region. Therefore the system remains metastable for larger value of supersaturation and this allows one to explore the high metastable region without encountering the KS. On increasing the range of interaction, both the critical cluster size and pre-critical minima in the free energy surface of kth largest cluster, at respective kinetic spinodals, shift towards smaller cluster size. In order to separate surface tension contribution to the increase in the barrier from other non-trivial factors, we introduce a new scaling form for surface tension and use it to capture both the temperature and the interaction range dependence of surface tension. Surprisingly, we find only a weak non-trivial contribution from other factors to the free energy barrier of nucleation.

© 2012 American Institute of Physics

Article Outline

  1. INTRODUCTION
  2. MODEL SYSTEM AND COMPUTATIONAL DETAILS
  3. DEPENDENCE OF THE FREE ENERGY BARRIER OF NUCLEATION AND THE KINETIC SPINODAL ON RANGE OF INTERACTION POTENTIAL
    1. Dependence of coexistence activities and surface tension on range of interaction potential
    2. Dependence of free energy barrier for nucleation on range of interaction potential
    3. Dependence of kinetic spinodal and size distribution of k th largest clusters on the range of interaction potential
  4. SCALING RELATIONSHIP BETWEEN SURFACE TENSION AND THE RANGE OF INTERACTION POTENTIAL
  5. SEPARATION OF SURFACE TENSION FROM OTHER (NON-TRIVIAL) CONTRIBUTIONS TO THE FREE ENERGY BARRIER OF NUCLEATION
  6. CONCLUSION

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KEYWORDS and PACS

Keywords

free energy, Lennard-Jones potential, nucleation, phase diagrams, surface tension

PACS

ARTICLE DATA

Digital Object Identifier
http://dx.doi.org/10.1063/1.3685835

PUBLICATION DATA

ISSN

0021-9606 (print)  
1089-7690 (online)

Publisher

$abstract.society.value is a Member of CrossRef American Institute of Physics

For access to fully linked references, you need to log in.
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