DOI: 10.1063/1.2888995. Argon nucleation: Bringing together theory, simulations, and experiment

Argon nucleation: Bringing together theory, simulations, and experiment

10.1063/1.2888995

Crossref journal-article

AIP Publishing

The Journal of Chemical Physics (317)

Abstract

We present an overview of the current status of experimental, theoretical, molecular dynamics (MD), and density functional theory (DFT) studies of argon vapor-to-liquid nucleation. Since the experimental temperature-supersaturation domain does not overlap with the corresponding MD and DFT domains, separate comparisons have been made: theory versus experiment and theory versus MD and DFT. Three general theoretical models are discussed: Classical nucleation theory (CNT), mean-field kinetic nucleation theory (MKNT), and extended modified liquid drop model-dynamical nucleation theory (EMLD-DNT). The comparisons are carried out for the area below the MKNT pseudospinodal line. The agreement for the nucleation rate between the nonclassical models and the MD simulations is very good—within 1–2 orders of magnitude—while the CNT deviates from simulations by about 3–5 orders of magnitude. Perfect agreement is demonstrated between DFT results and predictions of MKNT (within one order of magnitude), whereas CNT and EMLD-DNT show approximately the same deviation of about 3–5 orders of magnitude. At the same time the agreement between all theoretical models and experiment remains poor—4–8 orders of magnitude for MKNT, 12–14 orders for EMLD-DNT, and up to 26 orders for CNT. We discuss possible reasons for this discrepancy and the ways to carry out experiment and simulations within the common temperature-supersaturation domain in order to produce a unified picture of argon nucleation.

Bibliography

Kalikmanov, V. I., WÃ¶lk, J., & Kraska, T. (2008). Argon nucleation: Bringing together theory, simulations, and experiment. The Journal of Chemical Physics, 128(12).

Authors 3

V. I. Kalikmanov (first)
J. Wölk (additional)
T. Kraska (additional)

References 54 Referenced 53

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Dates

Type	When
Created	17 years, 4 months ago (March 25, 2008, 6:45 p.m.)
Deposited	2 years, 2 months ago (June 19, 2023, 9:14 p.m.)
Indexed	3 weeks, 1 day ago (July 30, 2025, 6:50 a.m.)
Issued	17 years, 4 months ago (March 25, 2008)
Published	17 years, 4 months ago (March 25, 2008)
Published Online	17 years, 4 months ago (March 25, 2008)
Published Print	17 years, 4 months ago (March 28, 2008)

Funders 0

None

BibTeX

@article{Kalikmanov_2008, title={Argon nucleation: Bringing together theory, simulations, and experiment}, volume={128}, ISSN={1089-7690}, url={http://dx.doi.org/10.1063/1.2888995}, DOI={10.1063/1.2888995}, number={12}, journal={The Journal of Chemical Physics}, publisher={AIP Publishing}, author={Kalikmanov, V. I. and Wölk, J. and Kraska, T.}, year={2008}, month=mar }

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  "abstract": "<jats:p>We present an overview of the current status of experimental, theoretical, molecular dynamics (MD), and density functional theory (DFT) studies of argon vapor-to-liquid nucleation. Since the experimental temperature-supersaturation domain does not overlap with the corresponding MD and DFT domains, separate comparisons have been made: theory versus experiment and theory versus MD and DFT. Three general theoretical models are discussed: Classical nucleation theory (CNT), mean-field kinetic nucleation theory (MKNT), and extended modified liquid drop model-dynamical nucleation theory (EMLD-DNT). The comparisons are carried out for the area below the MKNT pseudospinodal line. The agreement for the nucleation rate between the nonclassical models and the MD simulations is very good\u2014within 1\u20132 orders of magnitude\u2014while the CNT deviates from simulations by about 3\u20135 orders of magnitude. Perfect agreement is demonstrated between DFT results and predictions of MKNT (within one order of magnitude), whereas CNT and EMLD-DNT show approximately the same deviation of about 3\u20135 orders of magnitude. At the same time the agreement between all theoretical models and experiment remains poor\u20144\u20138 orders of magnitude for MKNT, 12\u201314 orders for EMLD-DNT, and up to 26 orders for CNT. We discuss possible reasons for this discrepancy and the ways to carry out experiment and simulations within the common temperature-supersaturation domain in order to produce a unified picture of argon nucleation.</jats:p>",
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