Tailoring the Properties of Ni(111)/Graphone Interfaces by Intercalation of Al and Na: A DFT Study
Round 1
Reviewer 1 Report
Reviewer report on the manuscript Journal of Carbon Research_C-1962759
Archana Ramakrishnan et al. “Tailoring the Properties of Ni(111)/Graphone Interfaces by Intercalation of Al and Na: A DFT Study”
In present manuscript, the monolayer of maximum coverage of Na and Al on the Ni (111) surface has been comparatively studied. Significant changes in magnetic and electronic properties at Ni(111)/graphone interface have been observed upon intercalation.
The manuscript can be accepted after minor revision. Authors should make the following corrections:
1. The introduction doesn’t provide sufficient background and include all relevant references. The references list should be extended and bring up-to date (2022) in this field. The 95% of references are older than 2015.
2. On page 1 of the manuscript is written: “The functionalization and dispersion of graphene sheets are crucial to their end applications [2].” The reference [2] is 11 years old (from 2011). It should be brought up-to date (2022). I recommend the publications [Carbon 2022, 196, 264], [ACS Nano 2021, 15, 12358] and [Small 2021, 17, 2104316] and references there.
3. On page 1 of the manuscript is written: “However, the sublattice imbalance causes instability in free-standing graphone, which mainly arises as carbon atoms of only one of the sublattice sheets of graphene is being adsorbed by hydrogen [5, 6]. This urged the researchers to study the hydrogen adsorption at various coverages for a better understanding of optimizing the magnetic and electronic properties as that finds an application in hydrogen storage [7].” It would be very useful to implement here the comparison with under publications in this field related to investigation of interaction of graphene mesh with hydrogen atoms, which were published later than 2012. I can recommend to include [J. Alloys Compd. 2019, 792, 713] and [J. Electron Spectrosc. Relat. Phenom. 2014, 196, 99] and check for other references there.
4. English language and style are fine spell check required.
5. The manuscript was formatted carelessly. It should be re-formatted.
6. The references list was formatted carelessly. It should be re-formatted.
7. Line 316, Author Contributions should be specified for all co-authors of the manuscript.
8. Scientific terminology, errors and typos should be corrected, e.g.:
Line 76, “arrangements” should be “sections”
Line 150, “Park, et al.” should be “Park et al.”
Line 152, “they find…” should be “they found”
Line 166, “in ig .4 …” should be “in fig . 4”
Line 176, “Next, we have adsorbed the graphene sheet on Ni(111)/Al surface (Ni(111)/Al/Gr).” should be “Next, the graphene sheet on Ni(111)/Al surface (Ni(111)/Al/Gr) have been adsorbed.”
Lines 190-191, “in ref 20…” should be “in reference [20]”
Line 239 “as shown in fig 3” should be “as shown in fig. 3”
Lines 309-310, “unique properties found can find proper utilization in devices” should be “?”
Line 324 (Reference 6), “mag in Gr by H adsorbates” should be “?”
Line 343 (Reference 16), “Vanderbilt D Rapid Communications Soft self-consistent pseudopotentials in a generalized eigenvalue formalism” should be “?”
Lines 321-322, 324, 330, 331-332, 337-338, 339-340, 341-342, 347-348, 349-350 (References 3, 5, 9, 10, 13, 14, 15, 20, 21), The pages should be added.
Comments for author File: 
Comments.pdf
Author Response
Response to Reviewer 1 Comments
- The introduction doesn’t provide sufficient background and include all relevant references. The references list should be extended and bring up-to date (2022) in this field. The 95% of references are older than 2015
Response 1: As per the reviewer’s comments the introduction has been rewriiten. The references have been added until 2021 as per your suggestions.
- On page 1 of the manuscriptis written: “The functionalization and dispersion of graphene sheets are crucial to their end applications [2].” The reference [2] is 11 years old (from 2011). It should be brought up-to date (2022). I recommend the publications [Carbon 2022, 196, 264], [ACS Nano 2021, 15, 12358] and [Small 2021, 17, 2104316] and references there.
Response 2: The recommended references have been added which follow the references number – 3, 6, 7.
- On page 1 of the manuscript is written: “However, the sublattice imbalance causes instability in free-standing graphone, which mainly arises as carbon atoms of only one of the sublattice sheets of graphene is being adsorbed by hydrogen [5, 6]. This urged the researchers to study the hydrogen adsorption at various coverages for a better understanding of optimizing the magnetic and electronic properties as that finds an application in hydrogen storage [7].” It would be very useful to implement here the comparison with under publications in this field related to investigation of interaction of graphene mesh with hydrogen atoms, which were published later than I can recommend to include [J. Alloys Compd. 2019, 792, 713] and [J. Electron Spectrosc. Relat. Phenom. 2014, 196, 99] and check for other references there.
Response 3: The references are incorporated as suggested. The reference numbers are 8 and 12.
- English language and style are fine spell check required.
Response 4: The spell check has been successfully done.
- The manuscript was formatted carelessly. It should be re-formatted.
Response 5: The manuscript has been re-formatted as per journal guidelines.
- The references list was formatted carelessly. It should be re-formatted.
Response 6: The reference list has been re-formatted as per the journal guidelines.
- Line 316, Author Contributions should be specified for all co-authors of the manuscript.
Response 7:
Author Contributions: Archana Ramakrishnan(AR): Conceptualization of the research idea, performing calculations, formal analysis and interpretation and drafting of the manuscript. Niharika Joshi(NJ): Formal analysis and interpretation of the investigations and drafting of the manuscript. The authors (AR and NJ) hold an equal contribution in the current research investigation Thirumalaiswamy Raja*: project supervision, reviewing and editing of the manuscript. All authors have read and agreed to the published version of the manuscript.
- Scientific terminology, errors and typos should be corrected, e.g.:
Response 8:
Line 76, “arrangements” should be “sections”
“The paper consists of the following sections: in the section below, the methodology of the work where the computational details have been elaborated.”
Line 150, “Park, et al.” should be “Park et al.”
“Park et al. [20] have considered different coverages ranging from 0.06 ML (0.16 ML by their definition) to 0.42 ML (1.07 ML by their definition).”
Line 152, “they find…” should be “they found”
“However, they found that the effect of intercalation of Na on graphene saturates after 0.25 ML (0.63 ML by their definition).”
Line 166, “in ig .4 …” should be “in fig . 4”
“This is also evident from the density of states plotted of Ni-d and Na-s in Fig. 4, where we observe negligible overlap between the Ni and Na states.”
Line 176, “Next, we have adsorbed the graphene sheet on Ni(111)/Al surface (Ni(111)/Al/Gr).” should be “Next, the graphene sheet on Ni(111)/Al surface (Ni(111)/Al/Gr) have been adsorbed.”
“Next, we have adsorbed the graphene sheet on Ni(111)/Al surface (Ni(111)/Al/Gr) have been adsorbed.”
Lines 190-191, “in ref 20…” should be “in reference [20]”
“In Ni(111)/Na(hcp)/Gr surface Gr is observed to be around 2.40 (4.76) Å away from the Na (top Ni(111)) layer, which is in perfect agreement with the reported distances [27] at 0.25 ML coverage.”
Line 239 “as shown in fig 3” should be “as shown in fig. 3”
“The rectification has been done according to the comment, “In the case of Ni(111)/Na/GrH, the hydrogenation of graphene favors a stable configuration at the fcc C of the graphone sheet, as shown in Fig. 3 (b); the distance between Na-C is 2.44 Å.”
Lines 309-310, “unique properties found can find proper utilization in devices” should be “?”
The rectified sentence for the comment is as follows :
“Thus, the intercalation of atoms between Ni(111) and graphone significantly plays a role in tuning the interface properties such that the unique properties can find its appropriate utilization to develop smart devices in spintronic or semiconductor applications.”
Line 324 (Reference 6), “mag in Gr by H adsorbates” should be “?”
The reference has been reformatted in the required format - Željko Šljivančanin, Richard Balog, Liv Hornekær, Magnetism in graphene induced by hydrogen adsorbates, Chem. Phys. Lett. 2012, 541, 70-74.
Line 343 (Reference 16), “Vanderbilt D Rapid Communications Soft self-consistent pseudopotentials in a generalized eigenvalue formalism” should be “?”
The reference has been formatted as - Vanderbilt, David, Communications Soft self-consistent pseudopotentials in a generalized eigenvalue formalism, Phys. Rev. B, 1990, 41, 7892-7895
Lines 321-322, 324, 330, 331-332, 337-338, 339-340, 341-342, 347-348, 349-350 (References 3, 5, 9, 10, 13, 14, 15, 20, 21), The pages should be added.
Page numbers are added to the above-mentioned references
Thankful for your valuable comments. The response to the reviewer's comments has been attached as a word document.
Author Response File: Author Response.pdf
Reviewer 2 Report
The research letter entitled "Tailoring the properties of Ni(111)/Graphone interfaces by intercalation of Al and Na: A DFT study" is gone through carefully and the comments on the manuscript are appended herewith. In this manuscript, the authors studied the nature of metal-graphone interaction, and tailoring the electronic and magnetic properties by introducing Al and Na. Based on density functional theory, this work calculates the stable structure, and analyzed the density of states. This work sounds very interesting and meaningful, and the analysis is reasonably clear. Therefore, it can be accepted for publication.
Author Response
Thanks for your acceptance of the manuscript.
Reviewer 3 Report
This manuscript is an intersting work. Some minor revisions are required before acceptance.
- The references style has to be unified according to that of C journal.
- Recent relevant refernces published in 2022 are recommended to be cited here.
Author Response
Thankful for your comments and valuable and worthy suggestions. The response for your comments are attached in the following word document.
Author Response File: Author Response.pdf
