Supercriticality, Glassy Dynamics, and the New Insight into Melting/Freezing Discontinuous Transition in Linseed Oil

Round 1

Reviewer 1 Report

The authors intended to study the change of broadband dielectric constant to investigate the supercriticality phenomenon as well as the melting/freezing discontinuous transition of linseed oil. Generally, the melting/fereezing was considered as the first-order phase transition (non-continuous phase transition), and the supercriticality is a continuous phase transition. I cannot found any study about  supercriticality in this maniscript. Besides, linseed oil is a natural product containing various fatty acid and therefore many kinds of fatty glyceride as well as many other components. Fatty glyceride is weak plar molecule. I doubt the accuracy of the measurement data in the oil study. So, I do not recommend that this study be published.

English is well written.

Author Response

1. The Reviewer:’I cannot found any study about  supercriticality in this maniscript (…) I doubt the accuracy of the measurement data in the oil study’.

The response: The supercritical behavior means the critical effect above the critical (or near–critical) effect described in agreement with the Physics of Critical Phenomena. Regarding the supercriticality applications, it should be evidenced particularly for dielectric constant.

Such results are clearly shown in Figures 2, 3, and subsequent (in the current version of the report; in the previous one they were Figures 1, 2, and subsequent) with clear description and justification in the text.

It means the conclusive statement of the Reviewer is in the strong disagreement with the report's merit, which means Not True, for me.

Nevertheless, I can also understand that the presentation is not clear enough for non-specialists. Hence, the end of the Introduction has been rewritten and the new comment explaining the basics of Critical Phenomena Physics and Supercriticality has been added before the Results and Discussion section.

2. The Reviewer:: ''I cannot find any study about supercriticality in this maniscript''

The response: I have reviewed hundreds of works and have never dared to make such an authoritarian statement without any justification.

It is also a completely untrue statement. For a final explanation of this issue, an extensive characteristic of the Novocontrol spectrometer was introduced at the beginning of the Methods & Discussion section. It wasn't done before because now it looks like an advertisement for superior features of the device and then the manufacturer.

But maybe for non-specialists, the parameters of the Novocontrol BDS impedance analyzer and Quattro unit are unknown. It is the world’s best Broadband Dielectric Spectrometer, well-known for any specialist in the given field, which is the source of the ‘experimental revolution’ in BDS studies.

It was enough to write 'Novocontrol' on the Internet to find the company's website.  All the extraordinary parameters can/could be noted immediately. The innovative methodology, distortions-sensitive, ‘is & was’, clearly referenced to the authors' papers.

The abstract has also been slightly changed to introduce readers to the concepts of supercriticality and premelting immediately.

I also draw attention to the Appendix showing experimental data and the 'Data Availability' statement clearly showing their Open Access availability (just after publication).

Reviewer 2 Report

Dear authors, its very interesting article, but a few things need to be corrected before publishing. The introduction should be enriched with a comparison of the research with the research of other scientists. Lines 510-536 from the Materials and Methods chapter should be moved to the Introduction. 

It is necessary to consider enriching the analysis of the obtained research results. Article written for the journal Biophysica or Int. J. Mol. Sci. 2021, 22? This information is on every page. Please correct!

Summary too extensive. Please definitely shorten them! The part about the research methodology and materials used in the experiment should not be placed after the part about the summary! please move this chapter after the introduction section.

Author Response

1. The Reviewer:  'The introduction should be enriched with a comparison of the research with the research of other scientists'

The response:  It has been done. Note the new part at the end of the Introduction where results of earlier dielectric studies in linseed oil and other vegetable oils are clearly specified. It is associated with 15 new references.

Such addition, suggested by the reviewer, led to the ‘revision’ of the end of the Introduction to present the target and results in frames of this ‘extended’ Introduction section.

2. The Reviewer: ‘ Lines 510-536 from the Materials and Methods chapter should be moved to the Introduction’.  

The Response: It has been done.

3. The Reviewer: ‘. Article written for the journal Biophysica or Int. J. Mol. Sci. 2021, 22? This information is on every page. Please correct’

The response:  The paper was written for the special invitation to Int. J. Mol. Sci. However, the editor advised the shift to Biophysica. I was not convinced, but finally agreed. This is the reason for this misprint. Now cleaned.

4.   The Reviewer: ‘ The part about the research methodology and materials used in the experiment should not be placed after the part about the summary! Please move this chapter after the introduction section. ‘

The response:  The structure of the paper follows the pattern advised for Int. J. Mol. Sci (the original submission).  I agree that this section just after the Introduction is always better. It has been shifted. Note that it is associated with the re-numbering of Figures.

Finally, following the suggestion the Summary/Conclusions is shorter and clarified.

Reviewer 3 Report

The content of the article titled: " Broadband dielectric studies in linseed oil: Super critical and the New Insight into Melting/Freezing Discontinuous Transition " successfully studied the broadband dielectric in linseed oil. The results obtained are very interesting, but at the present time the author needs to edit and complete with the following recommendations:
+ In the introduction, it is necessary to add the latest results on broadband dielectric in linseed oil, add the latest documents from 2018 to present, documents older than 10 years can be removed and only Keep only necessary documents. In addition, it is necessary to analyze the relationship between dielectric and temperature extensively to clarify the role of dielectric on the phase transition process of linseed oil.
+ In the research method section, the author needs to provide the calculation formula related to the quantities to be calculated, the parameters of the model along with cited sources.
+ Why did the author choose linseed oil to study the influence of dielectrics on the phase transition process without using other materials for research?. With the content of the current manuscript, the author investigates the influence of many factors such as phase transition, temperature,... on the dielectric of flaxseed oil, requiring the author to rearrange the structure into 4 parts: introduction, research methods, results and discussion and conclusion, and change the title accordingly.
+ When the temperature changes, how does the dielectric change? Does it follow any rules? It is necessary to explain the nature of the crystallization process when changing the dielectric and experimental results are needed to confirm the accuracy of the results obtained.
+ The author needs to explain in detail the above issues, add more content to the article, the results obtained in the summary and conclusion to clarify the issue.
+ I advise the author to check style, plagiarism and English language to ensure the magazines requirements.

Minor editing of English language required

Author Response

1.   The Reviewer: ‘In the introduction, it is necessary to add the latest results on broadband dielectric in linseed oil, add the latest documents from 2018 to present, documents older than 10 years can be removed and only Keep only necessary documents.   ‘

The response: It has been done. Note the new part at the end of the Introduction where results of earlier dielectric studies in linseed oil and other vegetable oils are clearly specified. It is associated with 15 new references.

Such addition, suggested by the Reviewer, led to the ‘revision’ of the end of the Introduction to present the target and results in frames of this ‘extended’ Introduction section.

2.   The Reviewer: ‘  In addition, it is necessary to analyze the relationship between dielectric and temperature extensively to clarify the role of dielectric on the phase transition process of linseed oil.

The response: Please note that such behavior constitutes the most important part of the results presented. In fact, all Figures presented in the Results section are related to the temperature behavior with the parameterization presented in the text via the subsequent equations.

I understand that the reviewer's comment means that the discussion in the text should be clarified. Such supplementary commenting has been done in the Results section.

Please note that the given report shows the first  (ever) functional discussion of pretransitional features in any vegetable oil, both for static and dynamic dielectric properties. 

3.   The Reviewer: ‘ In the research method section, the author needs to provide the calculation formula related to the quantities to be calculated, the parameters of the model along with cited sources ‘

The response:  Please note the first part of  [2. Methods and Materials] section where all discussed properties are precisely defined. For the model discussion in the Results section applied relations are clearly defined via Eqs. 5-15.

In the Appendix, all experimental data are presented. It includes the indication of relevant domains in dielectric studies, namely the LF domain, the static domain, the relaxation domain, and the DC-electric conductivity domain.

In the authors' opinion, all these offer a complete and well-defined picture. The style and grammar test of the text additionally clarified all issues.

4.   The Reviewer: ‘ Why did the author choose linseed oil to study the influence of dielectrics on the phase transition process without using other materials for research?. With the content of the current manuscript, the author investigates the influence of many factors such as phase transition, temperature,... on the dielectric of flaxseed oil, requiring the author to rearrange the structure into 4 parts: introduction, research methods, results and discussion and conclusion, and change the title accordingly.’

The response: With such a broad analysis of experimental data based on BDS research, with the support of innovative distortions-sensitive and derivative-based analysis, results regarding other vegetable oils would still defocus results. The work structure is now as suggested. We do not believe that we are examining the 'influence of many factors'. This work is rather a more complete use of BDS spectrum data, with an in-depth analysis that is probably already a standard in glass transition and critical phenomena physics - and unfortunately still not used not only for vegetable oils, but also for soft biomaterials more broadly. We hope this work will also indicate new possible research standards for BDS research in such materials.

The choice of linseed/flax oil was obvious due to its unique properties known for millennia (see Introduction) as well as its increasing applications today in a world of an increasingly ecological and sustainable economy. However, the fundamental insight into its properties is surprisingly limited and connects everything only to the properties of individual components. This work shows that there may be another – effective and collective – factor: supercriticality.

5.   The Reviewer: ‘ When the temperature changes, how does the dielectric change? Does it follow any rules? It is necessary to explain the nature of the crystallization process when changing the dielectric and experimental results are needed to confirm the accuracy of the results obtained.’

The response: The Results section is devoted entirely to this problem (Figs. 2-11) and Eqs. 5-11. It refers to two 'separate' - but, as it turns out, partially interactive - issues. Namely (i) pre-transitional effects in the liquid phase, which turn out to display surprisingly model features of weakly discontinuous phase transitions, i.e., a phenomenon in the field of Critical Phenomena Physics, (ii) Premeltig/post-freezing effect in the solid phase which is directly related to the mentioned crystallization and to the grand challenge of melting/freezing discontinuous transition. We understand the reviewer's comment that these issues should be better identified and separated, and we have improved the editing of the Results and Conclusions sections in this direction.

6.   The Reviewer:  ‘ I advise the author to check style, plagiarism and English language to ensure the magazines requirements’.

The response: Any plagiarism is obviously impossible for such new findings, based on the first-ever such class measurements & analysis in the given type of materials. The style and language have been tested, including the fit to Biophysica requirements.

Round 2

Reviewer 1 Report

The manuscript was well revised. It is acceptable in present form.

Reviewer 3 Report

The author has fully answered the requirements, I accept the manuscript content to be published online. 

Before publishing online, authors are asked to carefully check their style, English grammar and plagiarism one last time to ensure the magazines requirements without having to respond to reviewers. 

Congratulations on the success of the author's.

Minor editing of English language required