Quantum Monte Carlo and Density Functional Theory Study of Strain and Magnetism in 2D 1T-VSe2 with Charge Density Wave States

Daniel Wines; Akram Ibrahim; Nishwanth Gudibandla; Tehseen Adel; Frank M. Abel; Sharadh Jois; Kayahan Saritas; Jaron T. Krogel; Li Yin; Tom Berlijn; Aubrey T. Hanbicki; Gregory M. Stephen; Adam L. Friedman; Sergiy Krylyuk; Albert V. Davydov; Brian Donovan; Michelle E. Jamer; Angela R.Hight Walker; Kamal Choudhary; Francesca Tavazza; Can Ataca

doi:10.1021/acsnano.4c15914

Quantum Monte Carlo and Density Functional Theory Study of Strain and Magnetism in 2D 1T-VSe₂ with Charge Density Wave States

Daniel Wines
, Akram Ibrahim
, Nishwanth Gudibandla
, Tehseen Adel
, Frank M. Abel
, Sharadh Jois
, Kayahan Saritas
, Jaron T. Krogel
, Li Yin
, Tom Berlijn
, Aubrey T. Hanbicki
, Gregory M. Stephen
, Adam L. Friedman
, Sergiy Krylyuk
, Albert V. Davydov
, Brian Donovan
, Michelle E. Jamer
, Angela R.Hight Walker
, Kamal Choudhary
, Francesca Tavazza

Can Ataca

Research output: Contribution to journal › Article › peer-review

1 Scopus citations

Abstract

Two-dimensional (2D) 1T-VSe₂ has prompted significant interest due to the discrepancies regarding alleged ferromagnetism (FM) at room temperature, charge density wave (CDW) states, and the interplay between the two. We employed a combined Diffusion Monte Carlo (DMC) and density functional theory (DFT) approach to accurately investigate the magnetic properties, CDW states, and their responses to strain in monolayer 1T-VSe₂. Our calculations show the delicate competition between various phases, revealing critical insights into the relationship between their energetic and structural properties. We performed classical Monte Carlo simulations informed by our DMC and DFT results and found the magnetic transition temperature (T_c) of the undistorted (non-CDW) FM phase to be 228 K and the distorted (CDW) phase to be 68 K. Additionally, we studied the response of biaxial strain on the energetic stability and magnetic properties of various phases of 2D 1T-VSe₂ and found that small amounts of strain can increase the T_c, suggesting a promising route for engineering and enhancing magnetic behavior. Finally, we synthesized 1T-VSe₂ and performed Raman spectroscopy measurements, which were in close agreement with our calculated results, validating our computational approach. Our work emphasizes the role of highly accurate DMC methods in advancing the understanding of monolayer 1T-VSe₂ and provides a robust framework for future studies of 2D magnetic materials.

Original language	English
Pages (from-to)	9925-9935
Number of pages	11
Journal	ACS Nano
Volume	19
Issue number	10
DOIs	https://doi.org/10.1021/acsnano.4c15914
State	Published - Mar 18 2025

Funding

This work was supported by the National Science Foundation through the Division of Materials Research under NSF Grant No. DMR-2213398 and the Department of Energy (DOE) under Grant DE-SC0024236. The authors thank the National Institute of Standards and Technology for funding, computational, and data-management resources. Work by N.G. was supported by the National Institute of Standards and Technology Summer Undergraduate Research Fellowship program. Work by K.S. and J.T.K. (discussion, analysis of QMC calculations) was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division, as part of the Computational Materials Sciences Program and Center for Predictive Simulation of Functional Materials. Work by T.B. (discussion, analysis of DFT + U calculations) was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division. F.M.A. and B.D. would like to acknowledge the support of Peter Morrison and the Office of Naval Research under Contract No. N00014-21-WX-01248. Research at the United States Naval Academy (M.E.J.) was supported by the Office of Naval Research under Contract No. N0001423WX02132.

Keywords

2D magnets
2D materials
density functional theory
quantum Monte Carlo
strain
strongly correlated materials

Access to Document

10.1021/acsnano.4c15914

Cite this

Wines, D., Ibrahim, A., Gudibandla, N., Adel, T., Abel, F. M., Jois, S., Saritas, K., Krogel, J. T., Yin, L., Berlijn, T., Hanbicki, A. T., Stephen, G. M., Friedman, A. L., Krylyuk, S., Davydov, A. V., Donovan, B., Jamer, M. E., Walker, A. R. H., Choudhary, K., ... Ataca, C. (2025). Quantum Monte Carlo and Density Functional Theory Study of Strain and Magnetism in 2D 1T-VSe₂ with Charge Density Wave States. ACS Nano, 19(10), 9925-9935. https://doi.org/10.1021/acsnano.4c15914

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title = "Quantum Monte Carlo and Density Functional Theory Study of Strain and Magnetism in 2D 1T-VSe2 with Charge Density Wave States",

abstract = "Two-dimensional (2D) 1T-VSe2 has prompted significant interest due to the discrepancies regarding alleged ferromagnetism (FM) at room temperature, charge density wave (CDW) states, and the interplay between the two. We employed a combined Diffusion Monte Carlo (DMC) and density functional theory (DFT) approach to accurately investigate the magnetic properties, CDW states, and their responses to strain in monolayer 1T-VSe2. Our calculations show the delicate competition between various phases, revealing critical insights into the relationship between their energetic and structural properties. We performed classical Monte Carlo simulations informed by our DMC and DFT results and found the magnetic transition temperature (Tc) of the undistorted (non-CDW) FM phase to be 228 K and the distorted (CDW) phase to be 68 K. Additionally, we studied the response of biaxial strain on the energetic stability and magnetic properties of various phases of 2D 1T-VSe2 and found that small amounts of strain can increase the Tc, suggesting a promising route for engineering and enhancing magnetic behavior. Finally, we synthesized 1T-VSe2 and performed Raman spectroscopy measurements, which were in close agreement with our calculated results, validating our computational approach. Our work emphasizes the role of highly accurate DMC methods in advancing the understanding of monolayer 1T-VSe2 and provides a robust framework for future studies of 2D magnetic materials.",

keywords = "2D magnets, 2D materials, density functional theory, quantum Monte Carlo, strain, strongly correlated materials",

author = "Daniel Wines and Akram Ibrahim and Nishwanth Gudibandla and Tehseen Adel and Abel, \{Frank M.\} and Sharadh Jois and Kayahan Saritas and Krogel, \{Jaron T.\} and Li Yin and Tom Berlijn and Hanbicki, \{Aubrey T.\} and Stephen, \{Gregory M.\} and Friedman, \{Adam L.\} and Sergiy Krylyuk and Davydov, \{Albert V.\} and Brian Donovan and Jamer, \{Michelle E.\} and Walker, \{Angela R.Hight\} and Kamal Choudhary and Francesca Tavazza and Can Ataca",

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Wines, D, Ibrahim, A, Gudibandla, N, Adel, T, Abel, FM, Jois, S, Saritas, K , Krogel, JT, Yin, L, Berlijn, T, Hanbicki, AT, Stephen, GM, Friedman, AL, Krylyuk, S, Davydov, AV, Donovan, B, Jamer, ME, Walker, ARH, Choudhary, K, Tavazza, F & Ataca, C 2025, 'Quantum Monte Carlo and Density Functional Theory Study of Strain and Magnetism in 2D 1T-VSe₂ with Charge Density Wave States', ACS Nano, vol. 19, no. 10, pp. 9925-9935. https://doi.org/10.1021/acsnano.4c15914

TY - JOUR

T1 - Quantum Monte Carlo and Density Functional Theory Study of Strain and Magnetism in 2D 1T-VSe2 with Charge Density Wave States

AU - Wines, Daniel

AU - Ibrahim, Akram

AU - Gudibandla, Nishwanth

AU - Adel, Tehseen

AU - Abel, Frank M.

AU - Jois, Sharadh

AU - Saritas, Kayahan

AU - Krogel, Jaron T.

AU - Yin, Li

AU - Berlijn, Tom

AU - Hanbicki, Aubrey T.

AU - Stephen, Gregory M.

AU - Friedman, Adam L.

AU - Krylyuk, Sergiy

AU - Davydov, Albert V.

AU - Donovan, Brian

AU - Jamer, Michelle E.

AU - Walker, Angela R.Hight

AU - Choudhary, Kamal

AU - Tavazza, Francesca

AU - Ataca, Can

PY - 2025/3/18

Y1 - 2025/3/18

N2 - Two-dimensional (2D) 1T-VSe2 has prompted significant interest due to the discrepancies regarding alleged ferromagnetism (FM) at room temperature, charge density wave (CDW) states, and the interplay between the two. We employed a combined Diffusion Monte Carlo (DMC) and density functional theory (DFT) approach to accurately investigate the magnetic properties, CDW states, and their responses to strain in monolayer 1T-VSe2. Our calculations show the delicate competition between various phases, revealing critical insights into the relationship between their energetic and structural properties. We performed classical Monte Carlo simulations informed by our DMC and DFT results and found the magnetic transition temperature (Tc) of the undistorted (non-CDW) FM phase to be 228 K and the distorted (CDW) phase to be 68 K. Additionally, we studied the response of biaxial strain on the energetic stability and magnetic properties of various phases of 2D 1T-VSe2 and found that small amounts of strain can increase the Tc, suggesting a promising route for engineering and enhancing magnetic behavior. Finally, we synthesized 1T-VSe2 and performed Raman spectroscopy measurements, which were in close agreement with our calculated results, validating our computational approach. Our work emphasizes the role of highly accurate DMC methods in advancing the understanding of monolayer 1T-VSe2 and provides a robust framework for future studies of 2D magnetic materials.

AB - Two-dimensional (2D) 1T-VSe2 has prompted significant interest due to the discrepancies regarding alleged ferromagnetism (FM) at room temperature, charge density wave (CDW) states, and the interplay between the two. We employed a combined Diffusion Monte Carlo (DMC) and density functional theory (DFT) approach to accurately investigate the magnetic properties, CDW states, and their responses to strain in monolayer 1T-VSe2. Our calculations show the delicate competition between various phases, revealing critical insights into the relationship between their energetic and structural properties. We performed classical Monte Carlo simulations informed by our DMC and DFT results and found the magnetic transition temperature (Tc) of the undistorted (non-CDW) FM phase to be 228 K and the distorted (CDW) phase to be 68 K. Additionally, we studied the response of biaxial strain on the energetic stability and magnetic properties of various phases of 2D 1T-VSe2 and found that small amounts of strain can increase the Tc, suggesting a promising route for engineering and enhancing magnetic behavior. Finally, we synthesized 1T-VSe2 and performed Raman spectroscopy measurements, which were in close agreement with our calculated results, validating our computational approach. Our work emphasizes the role of highly accurate DMC methods in advancing the understanding of monolayer 1T-VSe2 and provides a robust framework for future studies of 2D magnetic materials.

KW - 2D magnets

KW - 2D materials

KW - density functional theory

KW - quantum Monte Carlo

KW - strain

KW - strongly correlated materials

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