General framework for nonclassical nucleation
A great deal of experimental evidence suggests that a wide spectrum of phase transitions occur in a multistage manner via the appearance and subsequent transformation of intermediate metastable states. Such multistage mechanisms cannot be explained within the realm of the classical nucleation framew...
| Main Authors: | , , , |
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| Format: | Article |
| Language: | English |
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IOP Publishing
2018-01-01
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| Series: | New Journal of Physics |
| Subjects: | |
| Online Access: | https://doi.org/10.1088/1367-2630/aad170 |
| _version_ | 1797750598216450048 |
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| author | Miguel A Durán-Olivencia Peter Yatsyshin Serafim Kalliadasis James F Lutsko |
| author_facet | Miguel A Durán-Olivencia Peter Yatsyshin Serafim Kalliadasis James F Lutsko |
| author_sort | Miguel A Durán-Olivencia |
| collection | DOAJ |
| description | A great deal of experimental evidence suggests that a wide spectrum of phase transitions occur in a multistage manner via the appearance and subsequent transformation of intermediate metastable states. Such multistage mechanisms cannot be explained within the realm of the classical nucleation framework. Hence, there is a strong need to develop new theoretical tools to explain the occurrence and nature of these ubiquitous intermediate phases. Here we outline a unified and self-consistent theoretical framework to describe both classical and nonclassical nucleation. Our framework provides a detailed explanation of the whole multistage nucleation pathway showing in particular that the pathway involves a single energy barrier and it passes through a dense phase, starting from a low-density initial phase, before reaching the final stable state. Moreover, we demonstrate that the kinetics of matter inside subcritical clusters favors the formation of nucleation clusters with an intermediate density, i.e. nucleation precursors. Remarkably, these nucleation precursors are not associated with a local minimum of the thermodynamic potential, as commonly assumed in previous phenomenological approaches. On the contrary, we find that they emerge due to the competition between thermodynamics and kinetics of cluster formation. Thus, the mechanism uncovered for the formation of intermediate phases can be used to explain recently reported experimental findings in crystallization: up to now such phases were assumed a consequence of some complex energy landscape with multiple energy minima. Using fundamental concepts from kinetics and thermodynamics, we provide a satisfactory explanation for the so-called nonclassical nucleation pathways observed in experiments. |
| first_indexed | 2024-03-12T16:36:06Z |
| format | Article |
| id | doaj.art-0d684f13a8fe4559be1b972ec4d273b1 |
| institution | Directory Open Access Journal |
| issn | 1367-2630 |
| language | English |
| last_indexed | 2024-03-12T16:36:06Z |
| publishDate | 2018-01-01 |
| publisher | IOP Publishing |
| record_format | Article |
| series | New Journal of Physics |
| spelling | doaj.art-0d684f13a8fe4559be1b972ec4d273b12023-08-08T14:52:21ZengIOP PublishingNew Journal of Physics1367-26302018-01-0120808301910.1088/1367-2630/aad170General framework for nonclassical nucleationMiguel A Durán-Olivencia0Peter Yatsyshin1Serafim Kalliadasis2https://orcid.org/0000-0001-9858-3504James F Lutsko3Complex Multiscale Systems Group, Department of Chemical Engineering, Imperial College London, London SW7 2AZ, United KingdomComplex Multiscale Systems Group, Department of Chemical Engineering, Imperial College London, London SW7 2AZ, United KingdomComplex Multiscale Systems Group, Department of Chemical Engineering, Imperial College London, London SW7 2AZ, United KingdomCenter for Nonlinear Phenomena and Complex Systems, Code Postal 231, Université Libre de Bruxelles , Blvd. du Triomphe, B-1050 Brussels, BelgiumA great deal of experimental evidence suggests that a wide spectrum of phase transitions occur in a multistage manner via the appearance and subsequent transformation of intermediate metastable states. Such multistage mechanisms cannot be explained within the realm of the classical nucleation framework. Hence, there is a strong need to develop new theoretical tools to explain the occurrence and nature of these ubiquitous intermediate phases. Here we outline a unified and self-consistent theoretical framework to describe both classical and nonclassical nucleation. Our framework provides a detailed explanation of the whole multistage nucleation pathway showing in particular that the pathway involves a single energy barrier and it passes through a dense phase, starting from a low-density initial phase, before reaching the final stable state. Moreover, we demonstrate that the kinetics of matter inside subcritical clusters favors the formation of nucleation clusters with an intermediate density, i.e. nucleation precursors. Remarkably, these nucleation precursors are not associated with a local minimum of the thermodynamic potential, as commonly assumed in previous phenomenological approaches. On the contrary, we find that they emerge due to the competition between thermodynamics and kinetics of cluster formation. Thus, the mechanism uncovered for the formation of intermediate phases can be used to explain recently reported experimental findings in crystallization: up to now such phases were assumed a consequence of some complex energy landscape with multiple energy minima. Using fundamental concepts from kinetics and thermodynamics, we provide a satisfactory explanation for the so-called nonclassical nucleation pathways observed in experiments.https://doi.org/10.1088/1367-2630/aad170nonlcassical nucleationphase transitionsfluctuating hydrodynamicsnucleation precursors |
| spellingShingle | Miguel A Durán-Olivencia Peter Yatsyshin Serafim Kalliadasis James F Lutsko General framework for nonclassical nucleation New Journal of Physics nonlcassical nucleation phase transitions fluctuating hydrodynamics nucleation precursors |
| title | General framework for nonclassical nucleation |
| title_full | General framework for nonclassical nucleation |
| title_fullStr | General framework for nonclassical nucleation |
| title_full_unstemmed | General framework for nonclassical nucleation |
| title_short | General framework for nonclassical nucleation |
| title_sort | general framework for nonclassical nucleation |
| topic | nonlcassical nucleation phase transitions fluctuating hydrodynamics nucleation precursors |
| url | https://doi.org/10.1088/1367-2630/aad170 |
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