Macroscopic nucleation phenomena in continuum media with long-range interactions

Nucleation, commonly associated with discontinuous transformations between metastable and stable phases, is crucial in fields as diverse as atmospheric science and nanoscale electronics. Traditionally, it is considered a microscopic process (at most nano-meter), implying the formation of a microscopic nucleus of the stable phase. Here we show for the first time, that considering long-range interactions mediated by elastic distortions, nucleation can be a macroscopic process, with the size of the critical nucleus proportional to the total system size. This provides a new concept of “macroscopic barrier-crossing nucleation”. We demonstrate the effect in molecular dynamics simulations of a model spin-crossover system with two molecular states of different sizes, causing elastic distortions.

[1]  O. Kahn,et al.  Spin-Transition Polymers: From Molecular Materials Toward Memory Devices , 1998 .

[2]  P. H. Lindenmeyer.  Surface area and secondary nucleation theory , 1977, Nature.

[3]  Suppression of capillary wave broadening of interfaces in binary alloys due to elastic interactions. , 2005, Physical review letters.

[4]  K. Ishida,et al.  Ferrous Polycrystalline Shape-Memory Alloy Showing Huge Superelasticity , 2010, Science.

[5]  A. C. Zettlemoyer,et al.  Homogeneous Nucleation Theory , 1974 .

[6]  S. Miyashita,et al.  Molecular dynamics study of thermal expansion and compression in spin-crossover solids using a microscopic model of elastic interactions , 2009 .

[7]  S. Miyashita,et al.  Simple two-dimensional model for the elastic origin of cooperativity among spin states of spin-crossover complexes. , 2007, Physical review letters.

[8]  John B. Goodenough,et al.  Magnetism and the chemical bond , 1963 .

[9]  P. Gütlich,et al.  Spin Crossover in Transition Metal Compounds II , 2004 .

[10]  John D. Dow,et al.  The Jahn-Teller effect in molecules and crystals , 1972 .

[11]  Effects of boundary conditions on magnetization switching in kinetic Ising models of nanoscale ferromagnets , 1996, cond-mat/9611054.

[12]  R. Baxter.  Exactly solved models in statistical mechanics , 1982 .

[13]  D. Frenkel,et al.  Onset of heterogeneous crystal nucleation in colloidal suspensions , 2004, Nature.

[14]  E. König.  Nature and dynamics of the spin-state interconversion in metal complexes , 1991 .

[15]  K. Kelton.  Crystal Nucleation in Liquids and Glasses , 1991 .

[16]  Renyi Zhang,et al.  Getting to the Critical Nucleus of Aerosol Formation , 2010, Science.

[17]  I. Bersuker,et al.  Modern aspects of the Jahn-Teller effect theory and applications to molecular problems. , 2001, Chemical reviews.

[18]  Savage,et al.  Kinetic pathway in Stranski-Krastanov growth of Ge on Si(001). , 1990, Physical review letters.

[19]  M. Lagally,et al.  Self-organization in growth of quantum dot superlattices. , 1996, Physical review letters.

[20]  W. Kurz,et al.  Fundamentals of Solidification , 1990 .

[21]  Isaac B. Bersuker,et al.  The Jahn-Teller Effect , 2006 .

[22]  W. Kurz,et al.  Fundamentals of Solidification: Fourth Revised Edition , 1998 .

[23]  J. Zimmer,et al.  Crystal symmetry and the reversibility of martensitic transformations , 2004, Nature.

[24]  A. Rappe,et al.  Nucleation and growth mechanism of ferroelectric domain-wall motion , 2007, Nature.

[25]  Max G. Lagally,et al.  KINETIC PATHWAY IN STRANSKI-KRASTANOV GROWTH OF Ge ON Si(001) , 1990 .

[26]  M. Bousquet-Mélou,et al.  Exactly Solved Models , 2009 .

[27]  A. Stancu,et al.  Cluster evolution in spin crossover systems observed in the frame of a mechano-elastic model , 2010 .

[28]  S. Miyashita,et al.  Realization of the mean-field universality class in spin-crossover materials , 2007, 0710.0921.

[29]  H. A. Jahn,et al.  Stability of Polyatomic Molecules in Degenerate Electronic States. I. Orbital Degeneracy , 1937 .

[30]  J. Schmelzer,et al.  Nucleation theory and applications , 1999 .

[31]  G. Meyrick,et al.  Phase Transformations in Metals and Alloys , 1973 .

[32]  Metastable lifetimes in a kinetic Ising model: Dependence on field and system size. , 1994, Physical review. E, Statistical physics, plasmas, fluids, and related interdisciplinary topics.

[33]  S. Miyashita,et al.  Intrinsic effects of the boundary condition on switching processes in effective long-range interactions originating from local structural change , 2010 .

[34]  A. Hauser,et al.  Cooperative phenomena and light-induced bistability in iron(II) spin-crossover compounds , 1999 .

[35]  J. Schmelzer.  Nucleation Theory and Applications: SCHMELZER:NUCLEATION O-BK , 2005 .