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Pressure-induced transitions in FePS$_3$: Structural, magnetic and electronic properties
by Shiyu Deng, Siyu Chen, Bartomeu Monserrat, Emilio Artacho, Siddharth S Saxena
This is not the latest submitted version.
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Submission summary
| Authors (as registered SciPost users): | Shiyu Deng |
| Submission information | |
|---|---|
| Preprint Link: | https://arxiv.org/abs/2209.05353v2 (pdf) |
| Date submitted: | Jan. 3, 2023, 4:29 p.m. |
| Submitted by: | Deng, Shiyu |
| Submitted to: | SciPost Physics |
| Ontological classification | |
|---|---|
| Academic field: | Physics |
| Specialties: |
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| Approach: | Computational |
Abstract
FePS$_3$ is a prototype van der Waals layered antiferromagnet and a Mott insulator under ambient conditions, which has been recently reported to go through a pressure-induced dimensionality crossover and an insulator-to-metal transition. These transitions also lead to the appearance of a novel magnetic metallic state. To further understand these emergent structural and physical properties, we have performed a first-principles study using van der Waals and Hubbard $U$ corrected density functional theory including a random structure search. Our computational study attempts to interpret the experimental coexistence of the low- and intermediate-pressure phases and we predict a novel high-pressure phase with distinctive dimensionality and different possible origins of metallicity.
Current status:
Has been resubmitted
Reports on this Submission
Report #2 by Anonymous (Referee 2) on 2023-3-9 (Invited Report)
- Cite as: Anonymous, Report on arXiv:2209.05353v2, delivered 2023-03-09, doi: 10.21468/SciPost.Report.6877
Strengths
Well-written work
Accurate ab-initio-based analysis
Potentially interesting results
Accurate ab-initio-based analysis
Potentially interesting results
Weaknesses
Introduction to be expanded
Number of figures elavated
Absence of theoretical modeling
Number of figures elavated
Absence of theoretical modeling
Report
By means of a first-principles study that uses van der Waals and Hubbard U corrected density functional theory including a random structure search the Authors try to understand how the external pressure tunes the dimensionality, structural, electronic and magnetic properties in FePS3. This numerical computational study attempts to interpret the experimental coexistence of the low- and intermediate-pressure phases and predicts a novel high-pressure phase with distinctive dimensionality and different possible origins of metallicity. A detailed study is also performed looking at the modifications induced by the interlayer sliding and dimensionality. The paper is interesting, well written and contains new results that deserve to be published. Nevertheless, before publication the following comments and remarks have to be properly addressed:
1. The references in the Introduction Section are thin on the ground and should be tailored to the subject at hand. Thus, I suggest enlarging this section mentioning recent papers.
See for instance for TMPX3 compounds:
Phys. Rev. Research 4, 023256 (2022); Phys. Rev. B 106, 035137 (2022); J. Phys. Chem. C 126, 6791 (2022); 2D Mater. 10, 014008 (2023); Phys. Rev. B 107, 075423 (2023).
See for instance for pressure-induced superconductors:
Nat. Commun. 5, 5508 (2014); Nat. Commun. 12, 5436 (2021); Proc. Natl. Acad. Sci.118, e2108938118 (2021); npj Quantum Mater. 7, 93 (2022); Nature 615, 244 (2023)
2. The explanation or some comments need to clarify the nature of the insulator-to-metal transition and how dimensionality is involved in the material under study.
3. Since the theoretical approach relies on DFT+U technique, I suggest to try an effort to theoretically model TXPX3, as done in some of the above mentioned papers.
1. The references in the Introduction Section are thin on the ground and should be tailored to the subject at hand. Thus, I suggest enlarging this section mentioning recent papers.
See for instance for TMPX3 compounds:
Phys. Rev. Research 4, 023256 (2022); Phys. Rev. B 106, 035137 (2022); J. Phys. Chem. C 126, 6791 (2022); 2D Mater. 10, 014008 (2023); Phys. Rev. B 107, 075423 (2023).
See for instance for pressure-induced superconductors:
Nat. Commun. 5, 5508 (2014); Nat. Commun. 12, 5436 (2021); Proc. Natl. Acad. Sci.118, e2108938118 (2021); npj Quantum Mater. 7, 93 (2022); Nature 615, 244 (2023)
2. The explanation or some comments need to clarify the nature of the insulator-to-metal transition and how dimensionality is involved in the material under study.
3. Since the theoretical approach relies on DFT+U technique, I suggest to try an effort to theoretically model TXPX3, as done in some of the above mentioned papers.
Requested changes
Introduction to be expanded
Theoretical model to be proposed
Report #1 by Anonymous (Referee 1) on 2023-3-6 (Invited Report)
- Cite as: Anonymous, Report on arXiv:2209.05353v2, delivered 2023-03-06, doi: 10.21468/SciPost.Report.6848
Strengths
1-Topic of broad interest
2-Very detailed analysis
3-Interesting results
2-Very detailed analysis
3-Interesting results
Weaknesses
1-Perhaps a little too long and redundant in some places
Report
The authors investigate the structural phases and electronic properties of FePS3 compound by means of density functional theory calculations. They perform a very detailed analysis of the system under pressure via a random structure search method to check what was found by experimental investigations and in order to predict possible new phases. With their investigation, the authors reproduce the known phases LP, HP-I and HP-II and they predict a new phase, namely HP-II-β . At ambient pressure the system is insulating, at pressure of around 14 GPa there is an inulator to metal transition, when the system changes structure from C2/m to P3 ̅1m in the HP-II phase. The new phase HP-II-β is predicted by the authors to be stable by means of phonon dispersion calculations. They also investigate the electronic properties and they present the evolution of the projected density of states as a function of the pressure and they show how the band gap becomes smaller at high pressures. The intra- or inter-layer P-P bonding affects the energy bands near the Fermi level, and might be responsible for a possibly different explanation for the origin of metallicity. The predicted dynamically stable HP-II-β phase defines a scenario for FePS3 turning metallic while becoming 3D-connected under high pressure. The magnetic moments on the transition metal atoms get suppressed when the system goes from the two-dimensional to three-dimensional limit.
I think the paper is well written and the results are interesting, I believe that it meets the acceptance criteria for publication as a SciPost article. The investigation of magnetism and structural properties of MPX3 compounds is a modern topic of great interest for applications and because these systems present metal to insulator transition and superconductivity phase too. These materials become fertile ground for exploring novel phases and emergent phenomena. Therefore I suggest the publication of this paper.
I think the paper is well written and the results are interesting, I believe that it meets the acceptance criteria for publication as a SciPost article. The investigation of magnetism and structural properties of MPX3 compounds is a modern topic of great interest for applications and because these systems present metal to insulator transition and superconductivity phase too. These materials become fertile ground for exploring novel phases and emergent phenomena. Therefore I suggest the publication of this paper.