Abstract
The field of 2D materials has grown dramatically in the past two decades. 2D materials can be utilized for a variety of next-generation optoelectronic, spintronic, clean energy, and quantum computing applications. These 2D structures, which are often exfoliated from layered van der Waals materials, possess highly inhomogeneous electron densities and can possess short- and long-range electron correlations. The complexities of 2D materials make them challenging to study with standard mean-field electronic structure methods such as density functional theory (DFT), which relies on approximations for the unknown exchange-correlation functional. To overcome the limitations of DFT, highly accurate many-body electronic structure approaches such as diffusion Monte Carlo (DMC) can be utilized. In the past decade, DMC has been used to calculate accurate magnetic, electronic, excitonic, and topological properties in addition to accurately capturing interlayer interactions and cohesion and adsorption energetics of 2D materials. This approach has been applied to 2D systems of wide interest, including graphene, phosphorene, MoS2, CrI3, VSe2, GaSe, GeSe, borophene, and several others. In this review article, we highlight some successful recent applications of DMC to 2D systems for improved property predictions beyond standard DFT.
| Original language | English |
|---|---|
| Article number | 031317 |
| Journal | Applied Physics Reviews |
| Volume | 12 |
| Issue number | 3 |
| DOIs | |
| State | Published - Sep 1 2025 |
Funding
This manuscript has been authored by UT-Battelle LLC under contract DE-AC05-00OR22725 with the U.S. Department of Energy (DOE). The U.S. government retains, and the publisher, by accepting the article for publication, acknowledges that the U.S. government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for U.S. government purposes. DOE will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan ( https://www.energy.gov/doe-public-access-plan ). This research used resources of the Argonne Leadership Computing Facility at Argonne National Laboratory, which is supported by the Office of Science of the U.S. Department of Energy, Office of Science, under contract number DE-AC02-06CH11357. D.W. acknowledges the National Institute of Standards and Technology for funding and support. J.A., A.B., P.R.C.K., J.T.K., L.M., B.R., and H.S. were 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 the Center for Predictive Simulation of Functional Materials. L.M. also received support (excitonic effects in 2D) from the U.S. National Science Foundation (Grant No. DMR-2316007). Y.K. was supported by the Basic Science Research Program (Grant No. 2018R1D1A1B07042443) through the National Research Foundation of Korea, funded by the Ministry of Education. I.S. acknowledges the support by APVV-21-0272, VEGA 2/0133/25, and VEGA 2/0131/23 and by the H2020 TREX GA 952165 projects and Funding by the EU NextGenerationEU through the Recovery and Resilience Plan for Slovakia (Project Nos. 09I02-03-V01-00012 and 09I05-03-V02-00055). K.S. and F.A.R. were supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division. C.A. acknowledges funding from the National Science Foundation (Grant No. NSF DMR-2213398) and the U.S. Department of Energy (Grant No. DE-SC0024236). Please note that certain equipment, instruments, software, or materials are identified in this paper to specify the experimental procedure adequately. Such identification is not intended to imply the recommendation or endorsement of any product or service by the National Institute of Standards and Technology, nor is it intended to imply that the materials or equipment identified is necessarily the best available for the purpose.