Toward improved property prediction of 2D materials using many-body
quantum Monte Carlo methods
Daniel Wines,
1, a)
Jeonghwan Ahn,
2
Anouar Benali,
3, 4
Paul R. C. Kent,
5
Jaron T. Krogel,
2
Yongkyung Kwon,
6
Lubos Mitas,
7
Fernando A. Reboredo,
8
Brenda Rubenstein,
9, 10
Kayahan Saritas,
2
Hyeondeok Shin,
11
Ivan
Štich,
12
and Can Ataca
13, b)
1)
Materials Science and Engineering Division, National Institute of Standards and Technology (NIST), Gaithersburg, MD 20899,
USA
2)
Materials Science and Technology Division, Oak Ridge National Laboratory, Oak Ridge, TN 37831,
USA
3)
Computational Science Division, Argonne National Laboratory, Argonne, IL 60439,
USA
4)
Qubit Pharmaceuticals, Incubateur Paris Biotech Santé, 24 rue du Faubourg Saint Jacques, 75014 Paris,
France
5)
Computational Sciences and Engineering Division, Oak Ridge National Laboratory, Oak Ridge, TN 37831,
USA
6)
Department of Physics, Konkuk University, Seoul 05029, Korea
7)
Department of Physics, North Carolina State University, Raleigh, NC 27695-8202, USA
8)
Material Science and Technology Division, Oak Ridge National Laboratory, Oak Ridge, TN 37831,
USA
9)
Department of Chemistry, Brown University, Providence, RI 02912, USA
10)
Department of Physics, Brown University, Providence, RI 02912, USA
11)
Computational Science Division, Argonne National Laboratory, Argonne, IL 60439,
USA
12)
Institute of Informatics, Slovak Academy of Sciences, 845 07 Bratislava, Slovakia
13)
Department of Physics, University of Maryland Baltimore County, Baltimore MD 21250
(Dated: 22 August 2025)
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, MoS
2
, CrI
3
, VSe
2
, 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.
1
I. INTRODUCTION
Since the synthesis of graphene in 2004 by Geim and
Novoselov that led to the 2010 Nobel Prize,
1–3
there has been
a)
Electronic mail: daniel.wines@nist.gov
b)
Electronic mail: ataca@umbc.edu
1
Notice: This manuscript has been authored by UT-Battelle LLC under con-
tract DE-AC05-00OR22725 with the US Department of Energy (DOE).
The US government retains and the publisher, by accepting the article for
publication, acknowledges that the US government retains a nonexclusive,
paid-up, irrevocable, worldwide license to publish or reproduce the pub-
lished form of this manuscript, or allow others to do so, for US govern-
ment purposes. DOE will provide public access to these results of feder-
ally sponsored research in accordance with the DOE Public Access Plan
(https://www.energy.gov/doe-public-access-plan).
an overwhelming interest in the field of 2D materials. 2D
materials are single-layer crystalline structures that have a
large lateral dimension compared to their thickness. Often-
times, these monolayers are exfoliated from layered materials
that are held together by weak van der Waals (vdW) bonds.
Due to their lack of surface groups or dangling bonds and
large surface-to-volume ratio, 2D materials can possess in-
teresting properties that are substantially different from those
of their bulk counterparts.
1–8
In addition, 2D materials can
possess enhanced quantum confinement and significantly re-
duced dielectric screening.
7–9
These materials also present
interesting phenomena such as enhanced carrier mobility,
1–3
reduction of charge carrier scattering,
1–6,9
superior mechani-
cal properties,
10
direct-to-indirect band gap transitions,
4
non-
trivial topological states,
11–13
and superconductivity
14,15
and
magnetism in 2D.
16
These physical phenomena can be ex-
ploited for future applications in optoelectronics, spintronics,
quantum computing, and clean energy.
17,18
In addition to graphene, there exist several other synthe-
