Variation along liquid isomorphs of the driving force for crystallization

Submission summary

 As Contributors: Nicholas Bailey Arxiv Link: http://arxiv.org/abs/1702.01010v2 (pdf) Date accepted: 2017-06-01 Date submitted: 2017-05-12 02:00 Submitted by: Bailey, Nicholas Submitted to: SciPost Physics Academic field: Physics Specialties: Condensed Matter Physics - Theory Statistical and Soft Matter Physics Approaches: Theoretical, Computational

Abstract

We investigate the variation of the driving force for crystallization of a supercooled liquid along isomorphs, curves along which structure and dynamics are invariant. The variation is weak, and can be predicted accurately for the Lennard-Jones fluid using a recently developed formalism and data at a reference temperature. More general analysis allows interpretation of experimental data for molecular liquids such as dimethyl phthalate and indomethacin, and suggests that the isomorph scaling exponent $\gamma$ in these cases is an increasing function of density, although this cannot be seen in measurements of viscosity or relaxation time.

Ontology / Topics

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Published as SciPost Phys. 2, 022 (2017)

We submit a revised version of our manuscript to SciPost Physics. We have made changes in several places in the paper in response to points raised by the reviewers. These consist mostly of additional text. The overall structure and the figures are unchanged. A few more changes are detailed below.

List of changes

1. The first subsection in section 1 starts now after the first paragraph, which now functions as a more overall introduction.
2. The term Roskilde (simple) liquid/system'' has been changeded to R-simple liquid/system'' to be consistent with current practice within the group.
3. A reference was added in the Introduction just before equation (1).
4. In appendix B we removed an unnecessary subscript on $\Delta \mu$.
5. A new appendix C has been added to clarify the derivation of Eq (22) (this was also requested by the second reviewer).
6. Minor re-writing of individual phrases and sentences.

Submission & Refereeing History

Resubmission 1702.01010v2 on 12 May 2017
Submission 1702.01010v1 on 6 February 2017

Reports on this Submission

Anonymous Report 1 on 2017-5-25 (Invited Report)

• Cite as: Anonymous, Report on arXiv:1702.01010v2, delivered 2017-05-25, doi: 10.21468/SciPost.Report.148

Strengths

1 - Well written and presented
2 - The article deepens our knowledge of the isomorphs
3 - The authors pertinently responded to the referees' requests and improved their work further

Weaknesses

1 - The article is of moderate impact.

Report

The authors have implemented most of the relevant changes requested by the referees and also pertinently replied to the questions raised.

In particular, it appears to me that the 2017-3-10 report missed the general scope of the article which is not to to provide a complete novel theory of crystallisation that includes its thermodynamic and kinetic aspects. More modestly, the article provides an insight on the thermodynamic driving forces for crystallisation from the point of view of the theory of isomorphs.

The authors replied rather clearly to the reports and improved the form of the presentation so that their aims are now clearer.

I would recommend publication at this stage.

Requested changes

None.

• validity: high
• significance: good
• originality: high
• clarity: high
• formatting: excellent
• grammar: excellent