DOI: 10.1063/1.4962166. Crystal nucleation as the ordering of multiple order parameters

Crystal nucleation as the ordering of multiple order parameters

10.1063/1.4962166

Crossref journal-article

AIP Publishing

The Journal of Chemical Physics (317)

Abstract

Nucleation is an activated process in which the system has to overcome a free energy barrier in order for a first-order phase transition between the metastable and the stable phases to take place. In the liquid-to-solid transition, the process occurs between phases of different symmetry, and it is thus inherently a multi-dimensional process, in which all symmetries are broken at the transition. In this Focus Article, we consider some recent studies which highlight the multi-dimensional nature of the nucleation process. Even for a single-component system, the formation of solid crystals from the metastable melt involves fluctuations of two (or more) order parameters, often associated with the decoupling of positional and orientational symmetry breaking. In other words, we need at least two order parameters to describe the free-energy of a system including its liquid and crystalline states. This decoupling occurs naturally for asymmetric particles or directional interactions, focusing here on the case of water, but we will show that it also affects spherically symmetric interacting particles, such as the hard-sphere system. We will show how the treatment of nucleation as a multi-dimensional process has shed new light on the process of polymorph selection, on the effect of external fields on the nucleation process and on glass-forming ability.

Bibliography

Russo, J., & Tanaka, H. (2016). Crystal nucleation as the ordering of multiple order parameters. The Journal of Chemical Physics, 145(21).

Authors 2

John Russo (first)
Hajime Tanaka (additional)

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Dates

Type	When
Created	8 years, 11 months ago (Sept. 13, 2016, 1 p.m.)
Deposited	2 years, 1 month ago (June 26, 2023, 4:23 a.m.)
Indexed	2 days ago (Aug. 19, 2025, 6:39 a.m.)
Issued	8 years, 11 months ago (Sept. 13, 2016)
Published	8 years, 11 months ago (Sept. 13, 2016)
Published Online	8 years, 11 months ago (Sept. 13, 2016)
Published Print	8 years, 8 months ago (Dec. 7, 2016)

Funders 1

Japan Society for the Promotion of Science 10.13039/501100001691
Region: Asia
gov (National government)
Labels6
1. KAKENHI
2. 日本学術振興会
3. Gakushin
4. JSPS KAKEN
5. JSPS Grants-in-Aid for Scientific Research
6. JSPS
Awards2
1. 25000002
2. 21224011

BibTeX

@article{Russo_2016, title={Crystal nucleation as the ordering of multiple order parameters}, volume={145}, ISSN={1089-7690}, url={http://dx.doi.org/10.1063/1.4962166}, DOI={10.1063/1.4962166}, number={21}, journal={The Journal of Chemical Physics}, publisher={AIP Publishing}, author={Russo, John and Tanaka, Hajime}, year={2016}, month=sep }

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  "abstract": "<jats:p>Nucleation is an activated process in which the system has to overcome a free energy barrier in order for a first-order phase transition between the metastable and the stable phases to take place. In the liquid-to-solid transition, the process occurs between phases of different symmetry, and it is thus inherently a multi-dimensional process, in which all symmetries are broken at the transition. In this Focus Article, we consider some recent studies which highlight the multi-dimensional nature of the nucleation process. Even for a single-component system, the formation of solid crystals from the metastable melt involves fluctuations of two (or more) order parameters, often associated with the decoupling of positional and orientational symmetry breaking. In other words, we need at least two order parameters to describe the free-energy of a system including its liquid and crystalline states. This decoupling occurs naturally for asymmetric particles or directional interactions, focusing here on the case of water, but we will show that it also affects spherically symmetric interacting particles, such as the hard-sphere system. We will show how the treatment of nucleation as a multi-dimensional process has shed new light on the process of polymorph selection, on the effect of external fields on the nucleation process and on glass-forming ability.</jats:p>",
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