1 s2.0 S0079642522001177 Main - Compressed 1

Progress in Materials Science 132 (2023) 101036
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Progress in Materials Science

journal homepage: www.elsevier.com/locate/pmatsci
Theory, properties and engineering of 2D magnetic materials

Shucheng Xing a, b, Jian Zhou a, b, Xuanguang Zhang a, b, Stephen Elliott a, b, c, d,
Zhimei Sun a, b, *
a
School of Materials Science and Engineering, Beihang University, Beijing 100191, China
b
Center for Integrated Computational Materials Engineering, International Research Institute for Multidisciplinary Science, Beihang University,
Beijing 100191, China
c
Department of Chemistry, University of Cambridge, Cambridge CB2 1EW, UK
d
Physical and Theoretical Chemistry Laboratory, University of Oxford, Oxford OX1 3QZ, UK
A R T I C L E I N F O A B S T R A C T
Keywords: Two-dimensional (2D) magnetism with a high Curie temperature (Tc) has been the pursuit of
2D magnetic materials generations for its potential application in spintronic devices. Meanwhile, some intriguing
Curie temperature physical properties, including the quantum anomalous Hall effect and skyrmions, have been
Machine learning
observed in 2D ferromagnetic materials (2DFMs), which are attractive for applications in high-
Symmetry breaking
Skyrmions
efficiency quantum and memory devices. However, the realization of 2D magnetism by experi
Quantum anomalous Hall effect ments has only been made in the last several years, but the Tc of these 2D materials is extremely
Magnetoelectric low. Therefore, the search for 2D intrinsic ferromagnetic materials with high values of Tc, or
Magneto-optics enhancing Tc by various modulation methods to inhibit thermal fluctuations, are current active
research directions. Here, we present a broad review of recent progress in 2DFMs. The physical
background is first illustrated as a prerequisite for a deep understanding of 2DFMs. 2DFMs can
have high values of Tc, and machine learning and high-throughput screening can play a vital role
in achieving this. Modulation methods to stabilize long-range magnetic order are emphasized
from the perspective of symmetry breaking. Finally, some distinctive properties of 2DFMs for
device applications are highlighted. The research directions that we propose here will be of great
assistance in exploring and understanding novel 2DFMs that can generate new devices in the
fields of spintronics and memory devices.
1. Introduction
Two-dimensional ferromagnetic materials (2DFMs), owing to their distinct characteristics, are considered as one of the most
promising solutions for next-generation spintronic devices in a revolution in semiconductor technology [1–5]. Great efforts have been
devoted to realize magnetism in 2DFMs since the first successful exfoliation of 2D van der Waals materials [4–6]. However, such
attempts to produce 2DFMs ended up in failure in the past decades. Why is the finding of magnetic low-dimensional materials so
difficult, when magnetism in bulk phases has been found thousands of years ago?
The existence of an ordered arrangement of magnetic moments over macroscopic length scales is the hallmark of magnetism in 2D
materials, driven by the coupling interaction between adjacent spins [7]. The spins favour specific orientations at zero temperature,
but they will increasingly misalign with increasing temperature owing to thermal fluctuations, which is essentially a spontaneous
* Corresponding author at: School of Materials Science and Engineering, Beihang University, Beijing 100191, China.
E-mail address: [email protected] (Z. Sun).
https://doi.org/10.1016/j.pmatsci.2022.101036
Received 15 August 2021; Received in revised form 25 September 2022; Accepted 17 October 2022
Available online 22 October 2022
0079-6425/© 2022 Elsevier Ltd. All rights reserved.
S. Xing et al. Progress in Materials Science 132 (2023) 101036
Nomenclature
2DFMs 2D ferromagnetic materials

AFM Antiferromagnetic
BKT Berezinskii-Kosterlitz-Thouless
BMS Bipolar magnetic semiconductor
Tc Curie temperature
COD Crystallography Open Database
Hc Coercive field
CGMD Crystal graph multilayer descriptor
CVD Chemical vapor deposition
DMS Dilute magnetic semiconductor
DMI Dzyaloshinskii–Moriya interaction
DFT Density-functional-theory
Gex Exchange gap
FGT Fe3GeTe2
FPS FePS3
FET Field-effect transistor
FM Ferromagnetic
FE Ferroelectric
GL Ginzburg-Landau
GKA Goodenough-Kanamori-Anderson
HTP High-throughput
HSCs Half-semiconductors
HM Half-metal
h-BN Hexagonal boron nitride
ICSD Inorganic Crystal Structure Database
MOFE Magneto-optical Faraday effect
MOKE Magneto-optical Kerr effect
ML Machine learning
MAE Magnetic anisotropy energy
MBE Molecular beam epitaxy
MFM Magnetic force microscopy
MPE Magnetic proximity effect
MOE Magneto-optical effect
NR Nanoribbon
OVL O-vacancy-line
QSL Quantum spin liquid
QAHE Quantum anomalous Hall effect
RKKY Ruderman–Kittel–Kasuya–Yosida
Ms Saturation magnetization
SOC Spin-orbit coupling
SGS Spin gapless semiconductor
SAW Surface acoustic wave
TMD Transition-metal dichalcogenide monolayer
TMX2 Transition metal dihalide
vdW Van der Waals
breaking of time-reversal symmetry [8]. The Mermin-Wagner theorem states that, for the isotropic Heisenberg model, continuous
symmetries cannot be spontaneously broken at finite temperatures in systems with sufficiently short-range interactions in dimensions
d ≤ 2, which is the reason for the difficulty in achieving long-range magnetic order in 2D systems [9]. A large magnetic anisotropy can
suppress random spin reorientations induced by thermal fluctuations, which provides a certain chance of finding 2D magnetic
behaviour. Recently, ground-breaking breakthroughs in producing 2D magnets have been achieved experimentally for CrI3 [10],
Cr2Ge2Te6 [11] and Fe3GeTe2 (FGT) [12]. Subsequently, intense experimental and theoretical investigations were devoted to
obtaining intrinsic magnetism in 2D materials without external modulation [13–15] which was what was mostly expected. However,
the Tc of current 2DFMs in experiments are too low to permit applications for room-temperature devices. Therefore, the search for 2D
magnetic materials with a large magnetic anisotropy energy (MAE) and a high Tc is a current research hotspot.
Emerging low-dimensional materials with extraordinary structures have aroused much interest; for instance, heterostructures,
Janus structures and nanoribbons show intriguing physical properties, such as the magnetic proximity effect and edge effects [16,17].
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Meanwhile, in order to improve the magnetic-anisotropy performance and the exchange-coupling strength, external control methods
to break the symmetry of the system have been utilized widely. Surface decoration [18–21], magnetic-atom doping [22–25] or the
application of electric fields [26,27] are prevailing methods to enhance Tc and the MAE. The material FGT is the most representative
example which exhibits room-temperature ferromagnetic order in tri-layer and four-layer samples under gate modulation [12]. Ma
chine learning (ML) with large datasets, either static or streaming, is one of the most rapidly growing core research fields that can be
applied effectively for discovering and predicting new materials, such as two-dimensional magnetic materials with high Tc. Hundreds
of magnetic films have been screened out by machine-learning models and high-throughput calculations [28–30].
In this review, we mainly aim to introduce the progress and principles of 2DFMs. We first review the development of a physical
theory for low-dimensional magnetism. Subsequently, some special and ‘hot’ materials are discussed. High-throughput (HTP) cal
culations and machine learning method for screening out 2DFMs with high Tc are introduced. We highlight the external control of
2DFMs by breaking the system symmetry to enhance the magnetic coupling. Some interesting physical phenomena, for instance
magnetoelectric effects, magneto-optics, the quantum anomalous Hall effect (QAHE) and skyrmions, are discussed as well. The
challenges and future prospects of 2D magnetic materials are concluded, including fundamental theory, synthesis and stability, flexible
spintronics and multiferroics.
2. Physical background
Before discussing low-dimensional magnetism, it is necessary to present a systematic overview of the development of the theory of
magnetism. In the following section, we start from the theory of spontaneous symmetry breaking and phase transitions to explain the
nature of ferromagnetic phase transitions. Then, we expound on the unique aspect of low-dimensional magnetism in terms of the
Mermin-Wagner theorem and seek a breakthrough point to enhance the magnetic exchange strength theoretically.
2.1. Spontaneously broken symmetries and phase transitions
Spontaneous symmetry breaking is defined as the phenomenon for any situation in physics in which the ground state of a system
has less symmetry than the system itself [8]. For instance, the ground state for magnetic iron is that the atomic spins are all aligned in
the same direction, bringing about a macroscopic magnetic field. A selected particular direction in space would break the rotational
symmetry of the system, while an increase in energy of the system can restore the symmetry but destroy the magnetic field [8].
Ferromagnetism, together with superfluidity and superconductivity, are examples of second-order phase transitions, in which the
symmetry may be reduced by the appearance of an ordered phase below a critical temperature [31]. Second-order phase transitions
exhibit a discontinuity in the second derivative of the free energy, which Landau first clarified by introducing order parameters [32].
Thereafter, the Ginzburg-Landau (GL) approach, based on the Landau second-order phase-transition theory, was proposed to interpret
superconductivity using a complex order parameter [33]. The GL approach can also be applied to describe ferromagnetic phase
transitions. Consider a model with a spin lattice and the coupling between the spins being along the X and Y directions (XY model),
( )
whose Hamiltonian is given by Equation (1). The order parameter is a 2D vector → m = mx , my and the formalism of the GL free energy
can be achieved by equation (2).
∑ ∑
H = − J Six Sjx − J Siy Sjy (1)
〈i,j〉〈i,j〉
∫
[ ]
F= d→
r ∂i →
m ∂i →
m + α→
m ⋅→
m + g(→
m ⋅→
m )2 + higher order terms (2)
where 〈i, j〉 represents the nearest-neighbors, J is the coupling constant and Sxi is the net spin at i site along x direction. α and g are
control parameters and → m is the order parameter.
However, the GL theory is a phenomenological theory, which cannot determine the value of the control parameters. During the
1960s, Wilson developed the renormalization group theory to analyse phase transitions, by which long-distance collective behaviour
was deduced by studying how the interaction parameters vary as length scales change [34]. It provides an accurate insight into the
mechanism of phase transitions and has been applied with success in many fields of physics, ranging from condensed matter to
quantum-field theory. Renormalization group theory achieved a satisfactory picture for the ferromagnetic transition and no phase
transition at a finite temperature of the Ising spin chain was demonstrated [31].
2.2. Mermin-Wagner theorem
The promise of low-dimensional materials, exploring the existence of intrinsic ferromagnetism, together with spontaneous sym
metry breaking, led to high expectations. Nonetheless, an important theorem, proposed by Mermin and Wagner [9], states that, at
finite temperatures, thermally activated fluctuations of Nambu-Goldstone modes destroy the long-range order, and thereby prevent
spontaneous symmetry breaking in one- and two-dimensional systems [9]. The Mermin-Wagner theorem therefore indicates that there
is no spontaneous magnetization in one and two dimensions for the isotropic Heisenberg model, as gapless spin-wave excitations can
be easily excited at any finite temperature. Nevertheless, the theorem is valid only for the isotropic Heisenberg model and is not
applicable even for a weak anisotropy, which creates a new way for seeking intrinsic low-dimensional ferromagnetic materials having
3
a sizeable magnetic anisotropy. Finally, it should be emphasized that the theorem is valid for arbitrary spin S and is restricted only to
the non-existence of spontaneous magnetization. The theorem does not necessarily exclude other types of phase transitions, for
example the divergence of the magnetic susceptibility [9].
2.3. Magnetic anisotropy
Magnetic anisotropy is the critical factor for 2DFMs as it prevents random spin reorientations induced by thermal fluctuations [35].
Generally, magnetic anisotropy mainly depends on two elements: spin–orbit coupling and magnetostatic dipole–dipole interactions,
which contribute to the magneto-crystalline anisotropy and shape anisotropy, respectively [36]. The concrete operator form of the
magnetic crystal anisotropy is determined by the symmetry group of the magnetic lattice. In principle, the magnetic anisotropy energy
is calculated as two kinds of differences in energy, namely the difference in the total energy, ΔEtot, with respect to two given directions
n1 and n2 of the magnetization, and the corresponding difference in the magnetic dipole–dipole interaction energy, ΔEdd. As the
magnetic dipole–dipole interaction is normally negligible for nanostructures [37], the magnetic anisotropy energy can be expressed as:
ΔEtot = Etot [n1 ] − Etot [n2 ] (3)
∫ ( )
1 2Zi
Etot (i) = Ec (i) + Ev (i) − dri ρ(ri ) V c (ri ) +
2 Ωi |ri |
∫ (4)
1
− Zi V inter (i) + dri ρ(ri )(∊xc [ρ(ri ) ] − V xc (ri ) )
2 Ωi
where Zi is the atomic number, and ρ(ri ) is the charge density.

∑
Ec (i) = ∊cj (i) (5)
j
∫ EF
Ev (i) = ni (z)∊dz (6)
↷
∫ ( ′)
2Zi ρ ri
(7)
′
V c (ri ) = − +2 ′ ⃒ dri
|ri | |ri − ri ⃒
⎡ ( ′) ⎤
∑ ∫ ρ rj Zj ⎦
(8)
′
V inter
(i) = 2 ⎣ drj ⃒ ⃒− ⃒ ⃒
j Ωj ⃒rj − r′ ⃒⃒ ⃒rj ⃒
j∕
=i j
The ∊cj (i) denotes the core one-electron energies corresponding to Ωi , and ni (z) is the density of states. The starting point of the
contour integral in Eq. (5) refers to the bottom of the valence-energy regime Eb. The term Ec (i) is usually called the core energy, Ev (i) is
the band energy, V c (ri ) is the Coulomb potential, and V inter (i) reflects the contribution of the intercell potential to the total energy.
∊xc [ρ(ri ) ] and V xc (ri ) are determined by the choice of a particular local spin-density functional [36].
Neglect of dipole–dipole interactions for the calculation of the magnetic-anisotropy energy, highly accurate electronic structures
and a strict treatment of the weak spin–orbit coupling (SOC) Hamiltonian are prerequisites for a reliable determination of EMAE for a
given material, which can be expressed as:
ħ →
Hso = p)⋅→
(∇ V × → σ (9)
4m20 c2
where V is the potential energy, p is the momentum, ħ is Plank’s constant, m0 is the mass of a free electron, c is the velocity of light,
and σ is the vector of Pauli matrices [38].
In low dimensions, the leading term in EMCA is the uniaxial anisotropy:
E = E0 + K2 sin2 θ + K4 sin4 θ (10)
where K is determined by the magnetic-force theorem and θ is the angle between the normal axis and the direction of magnetization
[39,40].
2.4. Magnetic coupling model
2.4.1. Heisenberg model

The Heisenberg model is considered to be the most extensively utilized and generally understood model of magnetism [41]. The
prerequisite of the model is the existence of permanent, localized moments, which interact with each other via either a direct or an
indirect exchange mechanism [41,42]. Therefore, the Heisenberg model is most suitable for magnetic insulators. Direct exchange in
the Heisenberg model is the exchange interaction that proceeds directly without the need for an intermediary. It generally plays a
minor role compared with other mechanisms in controlling the magnetic properties, as there is an insufficient overlap between
4
neighbouring magnetic orbitals. The Heitler-London method [43] has the advantage of giving a certain insight into the physical basis
for the direct exchange interaction, which can be manipulated for the hydrogen molecule. Indirect exchange can be further divided
into three categories: superexchange [44], double exchange [45] and the Ruderman-Kittel-Kasuya-Yosida (RKKY) interaction [46].
Superexchange is defined as an indirect exchange interaction between non-neighbouring magnetic ions. This semi-empirical law was
proposed to be named the Goodenough-Kanamori-Anderson (GKA) [47–49] rule to characterize superexchange interactions. The GKA
rule states that superexchange interactions are antiferromagnetic when the virtual electron transfer is between overlapping orbitals
that are each half-filled, but ferromagnetic when the virtual electron transfer is from a half-filled to an empty orbital or from a filled to
a half-filled orbital. The double exchange mechanism may arise between ions in different oxidation states, as first proposed by Zener
[45]. The double exchange mechanism occurs only when one atom has an extra electron compared to the other, which is different to
superexchange that arises between two atoms with the same valence. The RKKY interaction refers to a coupling mechanism of nuclear
magnetic moments, or localized inner d- or f-shell electron spins, in a metal by means of an interaction through the conduction
electrons [46]. Nevertheless, exact solutions available for the Heisenberg model are rare until now, so the appropriateness of the model
should be considered in any given situation.
2.4.2. Bond-dependent exchange (Kitaev model)

Bond-dependent exchange is crucial in low-dimensional materials for exotic many-body effects [50]. The Kitaev model, which
couples spin-1/2 degrees of freedom with bond-directional interactions, is an exactly solvable S = 1/2 spin model on a 2D honeycomb
lattice [51]. It has Ising-like couplings with a magnetic easy axis sensitive to the spatial orientation γ, whose Hamiltonian can be
written as:
∑
H= − Kγ Siγ Sjγ (11)
<ij>γ
where < ij>γ is a γ = x-type, y-type or z-type bond and the summation is taken over all honeycomb bonds, and Kγ is the bond-
indexed coupling constants [52,53]. In the Kitaev model, the nearest-neighbor spin degrees of freedom interact via strongly aniso
tropic Ising exchange, where the easy axis depends on the directions of the bonds or links. The Kitaev interactions along neighboring
bonds (x type, y type and z type) cannot be satisfied simultaneously, giving rise to “exchange frustration” and drives the system into a
quantum-spin-liquid (QSL) phase [54].The Kitaev spin model can be solved exactly using a fermionisation procedure which expresses
the spin-1/2 operators in terms of Majorana fermion operators, and the exact solution of the Kitaev model has a QSL ground state [51].
The Kitaev model can host a variety of both gapped and gapless QSL phases, based on the Ising model rather than Heisenberg in
teractions, depending on the underlying lattice and the spatial dimension. By mathematically replacing the spin operator Sγ (γ = x, y, z)
from the Kitaev Hamiltonian with two types of Majorana operators, bγ and c as Sγj = 2i bγj cj , the ground state can be described as an
ensemble of localized and itinerant Majorana fermions. For a bipartite lattice, in which all plaquettes contain an even number of bonds,
the Kitaev model has eigenvalues of ± 1, referring to zero (+1) or π (-1) flux [51,52]. It is straightforward to verify that all plaquette
operators commute with each other and with the Hamiltonian, thus describing integrals of motion. The conservation of this macro
scopic quantity allows one to greatly simplify the problem by limiting the discussion to a given flux sector [53].
2.4.3. Antisymmetric exchange interaction

The lack of inversion symmetry at interfaces or in non-centrosymmetric lattices induces the antisymmetric exchange interaction,
the so-called Dzyaloshinskii–Moriya interaction (DMI), which is an antisymmetric exchange interaction that can stabilize chiral spin
textures [55]. The Hamiltonian of the DMI interaction can be written as:
( )
(12)
(DM)
Hi,j = Dij ⋅ Si × Sj
in which Dij is the DMI vector with respect to the moments Si and Sj [56].
Anisotropic superexchange interactions are derived by extending the superexchange interaction theory to include spin–orbit
coupling effects [56]. The functional form of the DMI can be obtained through a second-order perturbative analysis of the spin–orbit
coupling interaction, between ions in Anderson’s superexchange formalism [49]. The form of Dij is closely related to the symmetry of
the crystal as well. The coupling between two ions in a crystal is considered first. Consider two points A and B which represent two ions
in the crystal, and denote the point where the line AB is bisected as C. When C is the center of inversion [56],
Dij = 0.
When a mirror plane perpendicular to AB passes through C,
Dij || mirror plane or Dij ⊥AB.
When there is a mirror plane including A and B,
Dij || mirror plane.
When a twofold rotation axis perpendicular to AB passes through C,
Dij ⊥ twofold axis.
When there is an n-fold axis (n ≥ 2) along AB,
Dij || AB.
DMI interactions favor the perpendicular orientation of chirality between two adjacent moments, competing with Heisenberg
exchange that tends to align parallel moments [57]. Large DMI interactions can also form chiral spin structures, such as chiral domain
5
walls [58], skyrmions [59] and quantum spin liquids [60], which are important for next-generation data-storage devices.
2.5. Layer-dependent effects
An interlayer exchange-coupled magnetic thin film is formed from multilayers, where two adjacent ferromagnetic layers are
coupled through a nonmagnetic spacer layer in between. This coupling is closely related to the oscillatory coupling, known as the
RKKY interaction, varying with the thickness of the spacer layer [46,61]. The interlayer exchange coupling has essentially the same
physical origin as the RKKY coupling between magnetic impurities in a nonmagnetic host, where the interfaces and impurities have
analogous effects on localized and spin-polarized disturbances, respectively. Several inchoate models of the interlayer exchange
coupling were based on a local-moment approximation explicitly using the RKKY interaction [62,63], while the validity for magnetism
in rare-earth multilayers and transition metals should be suspected with such an approximation. A free-electron approximation model
which is also qualitative, but contains much of the essential physics, was proposed in describing exchange-split bands in ferromagnetic
materials [64,65].
2.6. Fundamentals of symmetry breaking
2.6.1. Inversion symmetry breaking

A crystal with inversion symmetry implies that there is at least one center of symmetry making the crystal look the same as the
original under the operation of inversion symmetry:
r(x, y, z) → r(− x, − y, − z)
Out of the 32 point groups of crystals, 11 are centrosymmetric and 21 are non-centrosymmetric including 10 polar point groups. In
2D van der Waals (vdW) materials, inversion symmetry breaking is the root cause for many peculiar physical properties, such as
spin–orbit physics, Weyl fermions, valley-splitting effects, ferroelectricity and unconventional Ising superconductivity. The methods to
achieve inversion symmetry breaking include electric field [66], interlayer twisting [67], crystal phase control [68] and selectively
patterned adsorption [69].
2.6.2. Rotational symmetry breaking

Rotational symmetry implies that the crystal can coincide with itself after being rotated about its axis by a certain angle. Due to the
requirement of crystal periodicity, a crystal can only have 1-fold (C1), 2-fold (C2), 3-fold (C3), 4-fold (C4), and 6-fold (C6) rotational
symmetries. Rotational symmetry breaking can be fulfilled by the following methods: strain engineering [70], interlayer coupling [71]
and dimensionality reduction [72].
2.6.3. Time-reversal symmetry breaking

Time-reversal symmetry is the theoretical symmetry of physical laws under the transformation of time-reversal T: t → -t. The wave
function becomes complex conjugate under T: Tψ (r, t) = ψ * (r, − t) and the wave vector, k, of the Bloch state becomes -k under the
action of T. Thereafter, the physical properties at the wave vectors k and -k are linked by time-reversal symmetry. By breaking the time-
reversal symmetry, the degenerate states at K and K’ can be lifted, together with the appearance of various fascinating physical
phenomena, such as exotic spin excitations, quantum anomalous Hall, valley-splitting and magneto-optical effects. Time-reversal
symmetry breaking can be achieved by the following modulation methods in 2D materials: magnetic field [73], optical control
[74], magnetic-proximity effect [75], magnetic atom doping [24], surface functionalization and decoration [76].
2.6.4. Gauge symmetry breaking

Gauge symmetry in condensed-matter physics refers to the phase invariance of the wave function under the phase-transition
operation (ψ → eiαψ ). When the phase of the wave function changes, the gauge symmetry breaks, which underlies the existence of
exotic superfluids and superconductivity. Time-reversal symmetry breaking can be achieved by carrier doping [77] and flat-band
engineering [78].
3. Novel 2D ferromagnetic materials
Realizing remote magnetic ordering in low-dimensional systems was challenging, according to the Mermin-Wagner theorem, until
the first instances of intrinsic ferromagnetism were observed in CrI3 and Cr2Ge2Te6 down to the bilayer and monolayer limits. Both of
these materials are ferromagnetic insulators with low critical temperatures, Tc, for the phase transition (45 K for CrI3 monolayers and
28 K for Cr2Ge2Te6 bilayers) [10,11]. 2D Fe3GeTe2 was subsequently reported as a conductor with itinerant ferromagnetism, whose Tc
can be strongly modulated to room temperature by ionic gating [12]. Some other 2D magnetic materials have also been prepared
experimentally, including CrBr3 [79], CrSBr [80], MSe2 [81,82] (M = Mn, V), MnSn [83] and FeB2 (B = Se, Te) [68], by chemical-
vapor deposition and molecular-beam-epitaxy methods. Soon after this, great efforts were devoted to exploring the magnetization
in 2D materials by theoretical analysis, experimental synthesis and high-throughput screening together with machine learning. Some
previous reviews have systematically collated the newly-discovered 2D magnets based on their lattice symmetry (honeycomb,
triangular, square and rectangular lattices) [84] and number of elements (binary, ternary, multinary compounds) [85,86]. Here, we no
6
longer reintroduce these materials, instead we analyse some emerging systems and structures in low-dimensional magnetism,
including Janus structures, heterostructures, nanoribbons and MXenes/MBenes systems.
3.1. Janus structures
2D Janus materials are a newly derived form of 2D materials, where one type of atomic layer is replaced by another. Compared to
their prototypes, Janus materials display many intriguing properties by virtue of the structural symmetry breaking and built-in electric
field, such as large SOC [87], piezoelectricity [88] and valley polarization [17]. Tremendous efforts have been dedicated to detailed
investigations of their remarkable properties. 2D Janus materials have been demonstrated to exhibit significantly enhanced piezo
electric coefficients [89,90], easily induced intrinsic ferromagnetism [16,91] and advanced hydrogen-evolution reaction efficiencies
[92,93].
Novel characteristics of the Janus structures have significant effects on the long-range magnetic order of these two-dimensional
materials. In the research on magnetic properties of Janus structures, transition-metal dichalcogenide monolayers (TMDs) and 2D
transition-metal halides are the ‘hotspots’ which have been extensively reported in respect of valley polarization [17,91,94], enhanced
magnetic order [16] and strain-tunable-induced phase transitions [17,95–97]. Systematic investigations were implemented by Ren et
al. on Janus monolayers of VI3: V2Cl3I3 (VClI), V2Br3I3 (VBrI) and V2Cl3Br3 (VClBr), collectively called VXY materials (X, Y = Cl, Br and
I, X ∕
= Y). The competition between superexchange and direct exchange brings about the intrinsic ferromagnetism of VXY materials, as
demonstrated in Fig. 1a [16]. The enhanced ferromagnetism of Janus structures originates from the narrowed virtual exchange gap
(Gex). Gex decreases for CrI3, VI3 and VXY, respectively, which is consistent with the trend of Tc: Tc (VXY) > Tc (VI3) > Tc (CrI3). It is
worth noting that the Tc value of VXY is sensitive to strain, arising from the susceptibility of the exchange-coupling mechanism to
Fig. 1. (a) Schematic diagram of superexchange and direct exchange for monolayer VClI. (b) 2D Janus TMDs and induced polarization. (c) Planar
average of the electrostatic potential energy (navy-blue line) and planar average of the charge density (red line) perpendicular to the MoSSe surface.
Schematic of a field-effect spin-filter device and the I-VG relationships, based on the Janus material Cr2I3X3 (X = Br, Cl) monolayers under (d)
compressive strain and (e) tensile strain. ((a) reprinted with permission from Ref. [14] Copyright 2020 American Physical Society; (b) Ref. [59]
Copyright 2019 Royal Society of Chemistry; (c) Ref. [60] Copyright 2017 Royal Society of Chemistry; (d) (e) Ref. [61] Copyright 2019 Wiley). (For
interpretation of the references to colour in this figure legend, the reader is referred to the web version of this article.)
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deformation, and can be further elevated to 280 K by a tensile strain of 6% [16]. Apart from the long-range magnetic order, some other
intriguing characteristics have been investigated, such as the chiral spin texture in Janus CrXTe monolayers [97] and the Berezinskii-
Kosterlitz–Thouless (BKT) transition in vanadium-based Janus dichalcogenide monolayers [98].
Broken mirror symmetry and colossal vertical electric fields are the root causes of the novel magnetic features of the Janus
structures. Taking TMD single layers as an example, Cheng et al. first proposed the idea of breaking internal symmetry by predicting the
stability of polar monolayer TMDs [87]. Janus monolayer structures of TMDs are evolved from the complete replacement of one layer
of chalcogen atoms with another group VI element. The difference in the number of outermost valence electrons, between the top and
bottom layer elements, results in disparities of the electronegativity. This further brings about an asymmetric dipole distribution and a
colossal vertical electric field, depicted in Fig. 1b and c [99,100]. The point group of the monolayer changes simultaneously from D3h in
TMDs to C3v owing to the broken mirror symmetry.
The emergence of Janus structures has greatly enriched the research area of 2DFMs, and has repercussions, reflected in the
application to spintronic devices as well. The Janus Cr2I3X3 monolayers are bipolar magnetic semiconductors (BMSs) under a
compressive strain, while being half-semiconductors (HSCs) under a tensile strain. The strain-dependent electronic structure enables a
feasible approach to realize a half-metallicity in BMS/HSC structures simply by adjusting the position of the Fermi level, which can be
applied in the field-effect spin-filter device, shown in Fig. 1d and e [101]. An analogous phenomenon was found in VSeTe [17] which
undergoes a phase transition from BMS to a spin gapless semiconductor (SGS), HSC, half-metal (HM), and even a normal metal, under
biaxial strain. Simultaneously, a large valley polarization (169 meV) at the K and K’ reciprocal-lattice points of VSeTe was demon
strated, which was attributed to the breaking of both space and time-reversal symmetry by a large SOC effect [17]. Large valley
polarizations of Janus structures were also found in the Janus structure of 2H-VSeS [94] and could be implemented in applications for
valleytronics.
3.2. Heterostructures
Combining two kinds of 2D materials into heterostructures could regulate their overall performance [102–104], providing an
exotic platform to study interfaces and device applications with fascinating phenomena [105,106]. Two targets are being pursued to
form magnetic 2D materials as part of van der Waals heterostructures. One is expanding the functionality of the heterostructures
available for magnetic experiments and future device applications. The other is to investigate the magnetic properties of the heter
ostructures themselves, mainly originating from the proximity effect.
In the first place, vdW heterostructures can greatly broaden our horizons for seeking 2D ferromagnetic materials with high Tc and
Fig. 2. (a) Optical-microscopy image of Cr2Ge2Te6 flakes on a Si/SiO2 substrate. (b) Schematic of the layer structure of the device and electrical
connectivity and optical micrograph of the device, with MoSe2 and CrBr3 outlined in blue and green, respectively. (c) Left panel: the MOKE signal
measured on a different Cr2Ge2Te6 flake with similar thickness but thicker NiO (thickness 50 nm), showing an even stronger increase in the Curie
temperature to 115 K; Right panel: the MOKE signal measured on a relatively thick (202-nm-thick) Cr2Ge2Te6 flake with NiO with the same
thickness of 20 nm, showing an enhancement of the Curie temperature to 90 K. ((a) (c) reprinted with permission from Ref. [68] Copyright 2019
American Institute of Physics; (b) Ref. [68] Copyright 2020 Open Access Creative Commons Attribution 4.0 Licence). (For interpretation of the
references to colour in this figure legend, the reader is referred to the web version of this article.)
8
considerable uniaxial magnetic anisotropy. Since CrI3 and Cr2Ge2Te6 were first reported to exhibit ferromagnetism in 2D form [10,11],
researches on Cr2Ge2Te6 or CrI3-related heterostructures have become widespread. Great enhancements of Tc were simultaneously
demonstrated in 2D VI3/CrI3 [107], Cr2Ge2Te6/NiO [108] and Cr2Ge2Te6/PtSe2 [109] heterostructures. Based on density-functional-
theory (DFT) calculations, the MAE of Cr2Ge2Te6/PtSe2 is notably enhanced by 70%, and the Tc is increased far beyond room tem
perature [109]. An interlayer-distance-related magnetic anisotropy was discussed in graphene/NiI2 (Gr/NiI2) vdW heterostructures
[110]. The perpendicular magnetic anisotropy of NiI2 monolayers can be effectively strengthened via decreasing the interlayer dis
tance, which mainly originates from the electronic-state change of 5p orbitals of interfacial I atoms [110]. Simultaneously, the QAHE
can be induced in Gr/NiI2 via decreasing the interlayer distance, causing a range of Ueff values from 2 to 5 eV, as already demonstrated
in graphene-based heterostructures [111,112]. Magneto-optical Kerr effect (MOKE) measurements have been made under a
perpendicular magnetic field for the van der Waals ferromagnet, Cr2Ge2Te6, and its heterostructures formed with the antiferromag
netic (AFM) insulator, NiO [108]. A notable increase in both Tc and the magnetic perpendicular anisotropy were observed in
Cr2Ge2Te6/NiO heterostructures (Tc = 120 K) compared to Cr2Ge2Te6 monolayers (Tc = 60 K). Atomically thin flakes of Cr2Ge2Te6/
NiO heterostructures on Si/SiO2 substrates were visible via a thickness-dependent colour contrast due to interference effects, as shown
in Fig. 2a [108]. The jump in the ability to maintain long-range ferromagnetic order in Cr2Ge2Te6/NiO heterostructures can be realized
continuously with a variety of thicknesses, as demonstrated in Fig. 2c [108]. VdW AFM FePS3 (FPS) and FGT thin flakes were
fabricated to construct FPS/FGT and FPS/FGT/FPS heterostructures so as to improve the magnetic performance. Enhancements of Tc
and coercive field (Hc), of FGT were observed in both FPS/FGT and FPS/FGT/FPS heterostructures [113], as demonstrated by MOKE
results. This outstanding performance shows that AFM-FM coupling is an impressive way to strengthen itinerant ferromagnetism
without consuming any external energy [113].
The magnetic proximity effect (MPE) is naturally inevitable to take into consideration when coupling two materials with different
lattice arrangements together to form heterostructures [114,115]. Considering the interface formed by magnetic and non-magnetic
materials, the magnetic order of magnetic films can affect the properties of non-magnetic components and lead to new functional
ities [75]. MPE is one of the most essential interfacial phenomena in ferromagnet/superconductor heterostructures, [116,117] and
further is a pivotal approach to spin initialization for spintronics with the effects at the interface. Owing to the limited spread of the
electron wavefunction at the interface [118], the proximity effect is generally short-range, which can be widely exploited in vdW
materials with atomically thick and sharp interfaces [119,120].
In monolayer vdW materials, such as graphene or TMDs, even the range of short-range magnetic proximity effects exceeds their
thicknesses. The existence of an out-of-plane proximity-induced ferromagnetic exchange interaction was proved between graphene
and the magnetic insulator, Cr2Ge2Te6, by Karpiak et al [121]. A spin-lifetime anisotropy arises from the magnetic exchange, and SOC
was observed, which indicates the proximity-induced anisotropic spin texture in graphene [121]. The valley splitting induced by the
MPE was demonstrated in monolayer InSe, exerted by the ferromagnetic FeI2 substrate, which shows a strong distance-dependent
behavior with the interface distance [122]. A valley-splitting phenomenon is obtained as well in WSe2/CrI3 heterostructures by vir
tue of the inversion and time-reversal symmetry breaking and magnetic-proximity effects [123]. Engineering the interlayer distance
and the orientation of the substrate magnetic ordering can produce a modulation of the valley polarization and splitting energy [123].
The ferromagnetic insulator, CrBr3, induces strong spin polarization of graphene orbitals when formed into CrBr3-graphene hetero
structures [124]. Mini-band split-off energy gaps, together with an enhanced magnetic moment in the heterostructures, which is 8%
larger than that of the monolayer CrBr3 sheet, provides a platform for analysing the strong proximity correlation effect [124]. These
results suggest that MPE is intrinsically a localized effect that does not require specific interlayer stacking, and can be a good platform
for investigating exchange interaction effects.
The observation of the magnetic proximity effect from the perspective of experiment can mainly be achieved by polarization-
resolved photoluminescence [125], reflective magneto-circular dichroism [126], resonant optical spectroscopy [75] and the Zee
man spin Hall effect [119]. A layer-resolved magnetic proximity effect in heterostructures formed from monolayer WSe2 and bi/tri
layer CrI3 was discussed by utilizing the multiple magnetic configurations accessible in layered AFM CrI3 [126]. Individual exfoliated
WSe2 and CrI3 flakes were mechanically transferred to fabricate the WSe2/CrI3 heterostructures [126]. Polarization-resolved photo
luminescence and reflective magneto-circular dichroism experiments were utilized to investigate the relationship between the
proximity effect and magnetic states [126]. The proximity effect in MoSe2/CrBr3 heterostructures was discussed, synthesized by in
direct contact of monolayer MoSe2 and a bilayer of CrBr3 encapsulated in hexagonal boron nitride (h-BN) on an SiO2 substrate, as
depicted in Fig. 2b [75]. The valley Zeeman effect of MoSe2/CrBr3 heterostructures, demonstrated by the absence of itinerant hole
valley polarization, can be inferred to originate from the exchange coupling between conduction-band electrons in MoSe2 and CrBr3.
The electric-field dependence of the proximity effect, weak anisotropy of the exchange interaction and the critical exponents asso
ciated with the magnetic phase transition in MoSe2/CrBr3 heterostructures were revealed by employing resonant optical spectroscopy
[75]. Some other intriguing phenomena occur in heterostructures derived from magnetic-proximity effects, such as anomalous lon
gitudinal resistance changes [119], large values of magnetoresistance [127] and valley splitting and polarization in excitonic states
[128], which show the tremendous potential for spin/valleytronics.
3.3. Nanoribbons
One-dimensional structures have enhanced quantum-size effects and more special parameters for regulating their behaviour,
compared with 2D atomic-thick crystals, such as ribbon width [129], edge configuration [72] and tube diameter [130]. Probing the
properties of magnetism in nanoribbons (NRs) is intriguing for spintronic devices. CrI3 NRs and nanotubes were investigated at an
early stage [131–133] following the first experimental demonstration of intrinsic ferromagnetism in 2D CrI3. Wang et al. found that
9
CrI3 NRs remain in an FM state, regardless of the ribbon width, and the energy difference between the FM and AFM states can be
improved by even up to 3 to 4 times in zigzag NRs [131]. Guo et al. systematically investigated vanadium-trihalide VX3 (X = F, Cl, Br, I)
nanowires [134]. Finite-length, single-chain VI3 nanowires were demonstrated to be ferromagnetic semiconductors with a Tc around
64 K, while the other three halides (X = F, Cl, Br) are all antiferromagnetic [134].
Edge reconstruction and width regulation are prevailing methods to regulate the electronic and magnetic performance of NRs [72].
The magnetic moments and band gap of Janus MoSSe NRs and CrI3 NRs can be tuned by different non-metal atom passivation
[132,135]. A semiconductor-to-semimetal-to-metal transition is found to occur in graphene/h-BN hetero-NRs with an increase of the
width of the NRs [136]. Ti2CO2 MXene ribbons with an O-vacancy-line (OVL) defect have been investigated theoretically [137]. The
pristine Ti2CO2 ribbon is a nonmagnetic semiconductor, while significant magnetism can be induced by the presence of the OVL.
Enhanced magnetism was induced by mechano-electro-magnetic coupling effects due to further deformation at the ribbon edge upon
incorporation of the OVL [137]. Edge magnetic properties of black phosphorene NRs (Fig. 3a) have been investigated using static and
dynamical mean-field theory. The energy difference between AFM and FM phases is exponentially small, allowing a possible switch
between both states by tiny external fields [138]. In 1T’-MoS2 NRs (Fig. 3c), a ferromagnetic ground state can be stabilized by the edge
Fig. 3. (a) Three different magnetic spatial configurations for U/|t1| = 0.3 (left panel) and 1.0 (middle and right panels) of the Hubbard interaction
for black phosphorene nanoribbons. U/|t1| is the Hubbard interaction. The width and length of the ribbons are Nx = 7 and Ny = 120 units. (b) A
prototype information-storage device made of a single piece of MoS2 NR, which is composed of segments with different width (NZ) values (high or
low magnetic moments). The black arrows represent the spin polarization direction. (c) Edge reconstruction stabilizing an FM state at Mo edges. The
spin-charge distribution and relative total energy of the as-cut AS-NRs (NZ = 8) with the FM, NM, and AFM states at the Mo edge. (d) 5-AGNR
(armchair graphene nanoribbon) lifting experiments. (e) A: high-resolution STM image (5 mV, CO tip) of a doubly oxidized 14-UC 5-AGNR
(armchair graphene nanoribbon) on Au (1 1 1) (scale bar = 5 Å). B: high-resolution STM zoomed-in image of the oxidized end of the same nano
ribbon, showing the change in contrast at the edge of one ring. C: Suggested chemical structure for the oxidized GNRs. D: dI/dV line scan (oscillation
parameters of 731 Hz, 15 mV) of the same doubly oxidized nanoribbon. Both valence and conduction bands are visible, but there are no longer any
in-gap end states. ((a) reprinted with permission from Ref. [94] Copyright 2021 American Physics Society; (b) (c) Ref. [95] Copyright 2018
American Chemical Society; (d) (e) Ref. [96] Copyright 2020 American Chemical Society).
10
reconstruction arising from charge transfer from Mo atoms to the weaker Mo-S bonds next to the edges. The magnetic moment of 1T’-
MoS2 NRs intriguingly exhibits a periodic oscillation of between 0.1 and 1.2 µB with an increase of the NR width [72]. Inspired by this
discovery, a prototype information-storage device made of a single piece of MoS2 NR has been proposed, as illustrated in Fig. 3b [72].
Topological end states in 5‑armchair graphene NRs have been probed by scanning tunnelling spectroscopy measurements. Fig. 3d
describes the process of using this probe method to observe the tunnelling current to prove the magnetic nature of their topological end
states. To further determine which end state was being probed during the lifting, the ribbons at room temperature were exposed to
molecular oxygen [139]. The results shown in Fig. 3e demonstrate that no in-gap states are found in the doubly oxidized nanoribbon,
suggesting that the oxidation reaction results in the destruction of the end states [139]. In conclusion, one-dimensional nanoribbons,
compared with two-dimensional structures, have new adjustable degrees of freedom, such as band edge sites and nanoribbon widths.
Manipulation of these new tunable degrees of freedom can change their electronic structure and magnetic correlation, resulting in new
exotic properties.
Fig. 4. (a) Atomic structure of Cr2C. (b) Schematic of the exchange mechanism for Cr2CF2. The e1 and a orbitals of a Cr3+ ion are occupied in one
spin channel, and thus virtual hopping results in the AFM arrangement. (c) SEM image of Ti3C2Tx. (d) Magnetic moment (M) of as-prepared and
annealed MXene samples as a function of the applied field H, measured at 2 K. (e) M2xOxF2− x MXene models of Janus functionalization and collinear
magnetic ordering. Side, top, and bottom views of the supercell with the four termination sites labelled (top panel). Side views of the x = 1, x = 0.5,
and x = 1.5 models (middle panel). Collinear ferromagnetic (FM), intralayer antiferromagnetic (AFM1), and interlayer antiferromagnetic (AFM2)
ordering configurations are shown with spin-up (spin-down) in yellow (blue) (lower panel). (f) Schematic diagram of a synthesis process for MBenes.
((a) (b) reprinted with permission from Ref. [107] Copyright 2015 American Chemical Society; (c) (d) Ref. [110] Copyright 2020 Elsevier; (e)
Ref. [108] Copyright 2019 American Chemical Society; (f) Ref. [113] Copyright 2017 Royal Society of Chemistry). (For interpretation of the ref
erences to colour in this figure legend, the reader is referred to the web version of this article.)
11
3.4. MXenes/MBenes
3.4.1. MXenes
A fast-growing family of 2D materials, known as novel 2D transition-metal carbides, nitrides, and carbon nitrides (MXenes) were
introduced which have increased the enthusiasm for exploring their advanced features and promising applications [140]. The general
formula of MXenes is Mn+1XnTx, where M is an early transition metal (such as Sc, Ti, Zr, Hf, V, Nb, Ta, Cr, Mo, Mn), X is C and/or N, and
Tx in the formula represents the surface terminations (such as by O, OH, F, and/or Cl), and n = 1, 2, or 3. Selective acid etching of an A
layer from an MAX phase has been used to produce MXenes, a method which is superior to other approaches in aspects of control
lability, feasibility and cost efficiency [141]. Over 40 kinds of MXenes have been experimentally obtained, and many more have been
predicted according to theoretical analyses [142]. The richness of stoichiometry and surface functions endow 2D MXenes with highly
tailorable physical properties. The remarkable performance of MXenes in electronic (tunable bandgap, high electrical conductivity)
[143,144], mechanical (large elastic moduli) [145,146], optical [147,148] and electrochemical [149] applications have been amply
demonstrated.
Exploring the magnetic long-range order and spin transport of MXenes is a growing field in 2D materials to realize the application
for spintronics [150]. Since a large number of unpaired electrons exist in Cr and the first observation of long-range magnetic order was
made in Cr-based 2D materials, Cr2C has attracted extraordinary attention in the MXenes family for magnetic investigation, whose
structure is depicted in Fig. 4a [151]. Our group first demonstrated that Cr2C is a half-metallic ferromagnetic material among the
MXenes family [151]. An FM-AFM transition in Cr2C MXene has been observed, induced by surface functionalization with F, H, OH, or
Cl groups, which is accompanied by a metal-to-insulator transition. The underlying mechanism of the phase transition is induced by
the localization of Cr d electrons when Cr2C is functionalized [151]. A schematic of the exchange mechanism for Cr2CF2 is shown in
Fig. 4b. Furthermore, a search for stable long-range magnetic order in MXenes with a high Tc is always the goal of current research, and
significant achievements have already been widely reported, as listed in Table 1.
As Janus structures are endowed with advanced properties owing to the existence of built-in electric field and broken symmetry, an
upsurge in research on Janus-MXenes is occurring. Frey et al. studied the Janus structures of Mn2N, Cr2C, V2C, and Ti2C with
asymmetric surface functionalization, as depicted in Fig. 4e [76]. Mixed termination-induced anisotropy results in robust Ising
ferromagnetism, with an out-of-plane easy axis, for all models of mixed termination of Janus Mn2N materials. The Janus materials,
Cr2C, V2C and Ti2C, were found to be robustly antiferromagnetic [76]. Non-centrosymmetric structures can be stabilized by tuning the
interlayer exchange couplings with small applied electric fields, and enhanced bond directionality can be achieved by Janus func
tionalization, leading to improved magnetic anisotropy [76]. An intriguing phenomenon of FM-AFM co-existence was first reported in
La-doped Ti3C2Tx MXene, synthesized by a co-precipitation method [152]. This co-existence was demonstrated by the magnetization
vs temperature curves, ferromagnetic hysteresis loops and existence of exchange-bias, on account of the ferromagnetic orientation of
Table 1
Magnetic ground states, band structures, Curie/Neel temperatures for MXenes.
MXenes Magnetic Ground State Band Structure (eV) Tc/TN (K) Model Method
Cr2C FM Half-metallic (2.85) [151] 672 Heisenberg model GGA + U [369]

Cr2CO2 FM Metal [369] 695 Heisenberg model GGA + U [369]
Cr2CF2 AFM Semiconductor (3.49) [151] 2054 Heisenberg model GGA + U [369]
Cr2C(OH)2 AFM Semiconductor (1.43) [151] 2202 Heisenberg model GGA + U [369]
Zr2N AFM Semiconductor (1.5) [370] 470 2D Ising model GGA + U [370]
1T-Ti2C AFM Semiconductor (0.42 HSE06) [371] 50 Mean field GGA [372]
2H-Ti2C FM Half-metallicity (0.54 HSE06) [371] ~290 Heisenberg model GGA [371]
Fe2C FM Metal [373] 530 Heisenberg model GGA [373]
Co2C FM Metal [373] 130 Heisenberg model GGA [373]
Fe2CF2 FM Half-metal (0.66 HSE06) [373] 910 Heisenberg model GGA [373]
Fe2CO2 AFM Semiconductor (0.66 HSE06) [373] 40 Heisenberg model GGA [373]
Fe2C(OH)2 FM Half-metal (1.22 HSE06) [373] 220 Heisenberg model GGA [373]
Co2CF2 AFM Semiconductor (1.53 HSE06) [373] – – GGA [373]
Co2C(OH)2 AFM Semiconductor (1.12 HSE06) [373] – – GGA [373]
Ni2C AFM Metal [373] – – GGA [373]
Ni2CF2 AFM Semiconductor (0.51 HSE06) [373] – – GGA [373]
Mn2CF2 FM Half-metal (2.52 HSE06) [374] 520 2D Ising model PBE + U [374]
Mn2CO2 FM – 110 2D Ising model PBE + U [374]
Mn2C(OH)2 FM – 460 2D Ising model PBE + U [374]
Mn2CCl2 FM – 380 2D Ising model PBE + U [374]
Mn2CH2 AFM – 120 2D Ising model PBE + U [374]
Ti2MnC2O2 FM Semiconductor [375] 495 2D Ising model GGA + U [375]
Ti2MnC2(OH)2 FM – 1103 2D Ising model GGA + U [375]
Ti2MnC2F2 FM – 109 2D Ising model GGA + U [375]
Hf2MnC2O2 FM Semiconductor (0.238 GGA + U) [375] 829 2D Ising model GGA + U [375]
Hf2VC2O2 FM Semiconductor (0.055 GGA + U) [375] 1133 2D Ising model GGA + U [375]
Hf2MnC2(OH)2 AFM – – – GGA + U [375]
Hf2MnC2F2 AFM – – – GGA + U [375]
Hf2VC2(OH)2 AFM – – – GGA + U [375]
Hf2VC2F2 AFM – – – GGA + U [375]
12
titanium atoms along outer positions of the MXene sheets. To enhance the magnetism of Ti3C2Tx MXene, a method using H2 annealing
has been proposed [153]. An SEM image of Ti3C2Tx is shown in Fig. 4c. The saturation magnetization (Ms) of Ti3C2Tx gradually in
creases with increasing annealing temperature. The Ms in Ti3C2Tx-500 (the number denotes the annealing temperature) shows a
significant enhancement by about one order of magnitude, as depicted in Fig. 4d [153]. Furthermore, ordered double-transition-metal
MXene structures, such as Mo2TiC2Tx and Mo2Ti2C3Tx, have been experimentally realized, and more than twenty are theoretically
predicted, in which one or two layers of a transition metal are sandwiched between the layers of another one [154,155].
3.4.2. MBenes
Based on the development of MXenes, our group first proposed a new kind of 2D material, named 2D transition metal borons, whose
preparation process is shown in Fig. 4f [156]. Magnetic research on MBenes is rare, as their metallic nature limits the exploration of
ferromagnetic semiconductor or antiferromagnetic semi-metal properties for spintronics applications. Another aspect restraining the
development of MBenes is the difficulty of the synthesis. Nevertheless, a few papers focussing on the magnetic properties on MBenes
benefit from theoretical calculations [157,158]. Jiang et al. reported that 2D MnB sheets and their functionalized products exhibit
metallic ferromagnetic behaviour with the Tc above room temperature (345–600 K) [157]. A p–d hybridization mechanism and
Fig. 5. (a) Automated high-throughput machinery. The different building blocks of our end-to-end code for determining properties of 2DFMs, along
with an estimation of CPU and GPU usage of each block. (b) A full computational screening for magnetic 2D materials based on experimentally
known van der Waals bonded materials present in the crystal-structure databases ICSD and COD. (c) Figure of merit of the ferromagnetic semi
conductors identified through the computational screening, which combine adequate effective masses and Curie temperatures. (d) Illustration of the
crystal graph multilayer descriptor (CGMD). ((a) reprinted with permission from Ref. [126] Copyright 2020 Nature Publishing Group; (b) Ref. [127]
Copyright 2020 Nature Publishing Group; (c) Ref. [27] Copyright 2019 Nature Publishing Group; (d) Ref. [26] Copyright 2020 Wiley).
13
crystal-field splitting are the primary reasons leading to the nature of ferromagnetism and metallicity [157]. It is worth noting that the
vast majority of MBenes exhibit metallic properties; however, we recently reported that the transition from ferromagnetic metal to
antiferromagnetic semiconductor can be achieved through functional group adsorption on the surface of Cr2B2. The antiferromag
netism arises from interlayer superexchange interactions, while the intralayer interactions exhibit ferromagnetism [159]. Further
more, ferromagnetic semiconductor and ferromagnetic half-metallic states can be realized by nonuniform adsorption on both sides of
the Cr2B2 atomic layer, originating from the introduced built-in electric field [159]. Tetragonal phase Mn2B2 sheets with room-
temperature ferromagnetism and a sizeable MAE (out-of-plane magnetization axis) were then presented by Yusuf et al [160]. There
are relatively few studies on MBenes for spintronics at present, but a breakthrough in their experimental synthesis would break the
pattern in the future.
4. Machine learning and high-throughput search for 2D magnets
4.1. High-throughput search
High-throughput (HTP) computational materials design is an emerging field of materials science by generating, managing and
analysing enormous data warehouses to discover and designing novel materials, without their pre-synthesis [161–163]. High-
throughput methods greatly reduce the cost of the experiments and change the traditional way of performing DFT calculations,
from monitoring jobs on a few compounds to applying workflows applicable to thousands of compounds [164]. High-throughput
computations based on DFT have been applied to screen for various functional materials, such as thermoelectric [165], Li-air and
Li-ion batteries [166,167], electrocatalysts [168,169] and photovoltaic materials [170,171]. Herein, we systematically review and
explore the use of the HTP computational method in the search for 2D magnetic materials.
The high-throughput discovery of high Curie-point materials is the top priority of current research. Arnab et al. developed a fully
automated, hardware-accelerated, dynamic-translation-based computer code [172]. The workflow shown in Fig. 5a performs first-
principles-based computations, followed by Heisenberg-model-based Monte Carlo simulations to estimate the Tc. 26 materials with
a Tc beyond 400 K have been screened out from 786 materials by employing the code to conduct a high-throughput scan. An end-to-end
machine-learning model, with generalized chemical features through an exhaustive search of the model space as well as the hyper
parameters, was further adopted by using the scanned results. Using this algorithm, many important magnetic materials, involving
metals like Mo, W and Ti, were discovered which had so far been missed by heuristic-based formula-screening [172].
Daniele et al. proposed that, in the work of Arnab et al., introduced above, it is far from obvious that any of these materials can be
synthesized in the lab, even if DFT predicts them to be stable, since they are not derived from experimentally known van der Waals
bonded bulk compounds [173]. The team of Daniele performed a full computational screening for 2D magnetic materials based on
experimentally known van der Waals bonded materials present in the crystal-structure databases Inorganic Crystal Structure Database
(ICSD) and Crystallography Open Database (COD). 85 ferromagnetic and 61 antiferromagnetic materials were found with the
workflow depicted in Fig. 5b, in which 10 potentially exfoliable 2D ferromagnets were identified that had not been reported previously
[173]. In addition to the search for 2D magnetic materials, magnetic semiconductors combining strong ferromagnetism and superior
semiconducting properties are highly desirable for spintronic applications. Chen et al. first screened 15,300 semiconductors by
considering the thermodynamic stability (energy above the convex hull at 0 K lower than 50 meV per atom) and electronic band gap
(greater than 100 meV) [29]. Magnetic ordering of ~ 1000 compounds was estimated thereafter by comparing the total energies of the
ferromagnetic ground state to the antiferromagnetic or ferrimagnetic ones. The effective mass of electrons was mainly taken into
account when considering spintronic-device performance. However, it is challenging to simultaneously combine adequate air stability,
effective mass and Tc in a specific material. The material, In2Mn2O7, which was screened out, offers an exceptional compromise be
tween these three metrics and dopants and epitaxial strain to enhance the transport property and Tc, as shown in Fig. 5c [29]. Li et al.
presented a high-throughput investigation of the magnetic ground states for 90 transition-metal dihalide monolayers transition (TMX2)
using DFT, based on a collection of Hubbard U values [174]. The results show that 50 out of 55 magnetic TMX2 materials are more
stable in the 1T phase, except for FeX2 (X = Cl, Br and I) and TMX2 (X = Br and I), while the stable 2H phase is mainly adopted by
nonmagnetic TMX2 monolayers with a TM belonging to d1-d2 elements [174]. Han et al. attempted to extend the application of layered
double perovskites from optoelectronics to spintronics by the use of high-throughput discovery [175]. The results show that
Cs4MnSb2Cl12, Cs4CuSb2Cl12 and Cs4ScSb2Br12 with AFM ordering can be spintronic materials [175].
4.2. Machine learning
Machine learning (ML) is a branch of artificial intelligence (AI) in which algorithms are developed to generate models that can
predict or classify new input data autonomously [176]. Data-driven models combined with ML techniques can be more powerful,
capable of making predictions without prior knowledge of the system, and potentially achieving high accuracy at low computational
cost [177]. The main cores of machine learning are algorithms and data. The algorithms are divided into supervised learning and
unsupervised learning, including artificial neural networks [178], support vector machines [179] and random forest classification
[180]. Data for machine learning in the field of materials can be derived from existing databases, high-throughput computing or
experimental data. Utilizing adequate and accurate datasets with appropriate machine-learning methods is critical to the efficiency
and accuracy of machine-learning predictions.
In the field of 2D FM materials, methods combining advanced ML techniques with high-throughput density-functional-theory
calculations have been developed to form an adaptive framework for the acceleration of the discovery of 2D intrinsic FM materials. A
14
new crystal graph multilayer descriptor (CGMD) was proposed, depicted in Fig. 5d, using the elemental property to improve the
performance of ML models [26]. The accuracy of ML models with CGMD is over 90% in the challenging case of small-scale datasets.
Each layer of CGMD represents one elemental property of materials, such as atomic local environments and unpaired electrons. CGMD
is exactly a three-order tensor obtained by multiplying the atomic adjacency matrix by seven elemental feature matrices, respectively.
Thermodynamic stability, magnetic ground state, and bandgap classifications were carried out with the 2D material data and
descriptor by using the gradient-boosting classification algorithm. About 90 intrinsic FM materials with desirable bandgaps and
excellent thermodynamic stability were screened out, and a database containing 1459 2D magnetic materials was set up [26].
The distinction between different magnetic orders is another challenge for machine learning in the application of magnetic ma
terials, because, for antiferromagnetism, it has many configurations and is more complicated [181]. Long et al. subsequently developed
a FM/AFM classification model, along with a regression model, to predict the Tc values for intermetallic FM compounds, using the
random-forest method. These models were then used to identify the magnetic ground state of 5183 magnetic intermetallic compounds
[131]. Furthermore, Acosta et al. revealed that the magnetic ground state is closely related to the crystal structure, space group and
spin–orbit coupling of materials, by using a random-forest ML algorithm as well. The algorithm can precisely predict the magnetic
ground states, including NM, FM and AFM, with an accuracy as high as 90% [182].
Research on machine learning of magnetic materials is currently focused on efficiently predicting more low-dimensional magnetic
materials and magnetic ordering of magnetic materials [182]. However, studies of complex and intrinsic magnetic properties with ML
are relatively rare, such as magnetic-exchange interaction [183], magnetic topology [184] and skyrmions states [185]. Two aspects
restrict the application of ML for these complex and intrinsic magnetic properties: scarce data and complex physical correlations.
Different from basic electronic structure or magnetic ground states, the complex physical correlations, such as the magnetic-exchange
interaction, magnetic-topology states and Dzyaloshinskii–Moriya interaction [184] are more complicated and also harder to obtain by
calculation or experiment. Some attempts have been made to study the complex and intrinsic magnetic properties with ML method.
Estimation of magnetic Hamiltonian parameters using ML techniques was realized from magnetic-domain images, by generating a
large dataset of various spin configurations for ML processing. The datasets can show the magnetic-domain structures and the cor
responding magnetic Hamiltonian parameters [186]. The Dzyaloshinskii–Moriya interaction, as an antisymmetric exchange inter
action, is critical in inducing chiral magnetic order. The DM exchange constant can be estimated using pattern recognition and
machine learning, from a single image obtained in experiments [183]. 100,000 training images and 10,000 testing images with
different DM exchange constants were created using the micro-magnetic simulation code for the trained system. The trained system
can then be used to estimate the DM exchange constants and magnetic anisotropy energies from experimentally obtained magnetic-
domain images [183]. Nonetheless, machine-learning-based research in this area is still currently lacking; efficient and large-scale
high-throughput, computer-assisted, data-driven machine-learning methods are urgently needed to explore novel magnetic quan
tum properties in the future.
5. Modulation means for 2D magnets
The ferromagnetic materials studied at present mainly have inferior magnetic correlation strengths, whose macroscopic charac
teristic is a low Tc. In addition, MAE is a prerequisite for two-dimensional materials to have intrinsic magnetic order [35,36].
Therefore, improving the magnetic correlation and MAE in two-dimensional materials through some type of modification methods is a
research direction for realizing room-temperature magnetism in 2D materials. The currently widely used control methods mainly
include functional-group adsorption [21], defect structure [187], electric field [12], strain [97], alloying [188] and other orbital-
regulation means. Simultaneously, symmetry breaking is well-known as usually accompanying the emergence of fascinating phe
nomena. In 2D systems, integrating different broken symmetries can engender synergistic effects and promising phenomena in new
physics.
5.1. Time-reversal and spontaneous gauge-symmetry breaking
5.1.1. Magnetic atom and carrier doping

Dilute magnetic semiconductors (DMSs), realized by the substitutional doping of spin-polarized transition metals into semi
conducting systems, enable the experimental modulation of spin dynamics in ways that hold broad prospects for room-temperature
ferromagnetism and novel magnetoelectric or magneto–optical devices [22,189,190]. Doping of transition-metal elements, such as
Fe and Mn, into nonmagnetic bulk semiconductors, like p-type Mn-doped IV–VI [77], III–V [191,192], and II–VI [193,194] com
pounds, is known to facilitate the formation of DMSs. However, the main obstacles for obtaining high-temperature DMSs in experiment
are solubility and chemical stability when doping with transition-metal elements [195,196]. In order to break the above restrictions
and broaden research horizons, doping of transition-metal elements, such as V, Mn, and Fe, into two-dimensional materials to form
atomically thin DMSs, as a new attempt, would permit the exploration of the magnetic coupling in 2D confined structures [197,198].
Transition-metal dichalcogenides (TMDs) [7,171] have recently been of interest through the introduction of magnetic transition-
metal ions, such as V [199], Co [200], and Mn, [201] into the host lattice [22]. Ion doping is mainly achieved by two methods, namely
chemical vapour deposition [22,24,202] and powder vaporization [203]. The metal-precursor solution, prepared by mixing V and W
liquid sources in a given atomic ratio, is spin-coated onto SiO2 substrates introduced into the chemical vapor deposition chamber,
followed by selenization, producing a monolayer of VxW1− xSe2 [199]. The atomic ratio of vanadium to tungsten sources can be
precisely controlled from 0.1% to 40% in the precursor solution [199]. To confirm the presence of substitutional atoms at specific sites,
high-angle annular dark-field scanning transmission electron microscopy imaging is generally utilized. In addition, the microstructure
15
was also characterized, and unexpectedly few polyhedral aggregations were revealed [22,202,203]. The existence of magnetic order in
V-doped WSe2 monolayer was investigated by magnetic force microscopy (MFM), which can detect very small magnetic dipole mo
ments [199,204]. According to the MFM phases, it can be observed that there is no ferromagnetic order in pristine WSe2 with no
distinctive features (Fig. 6a), while the observation of the existence of large domains with phase contrast, separated by domain walls,
in 0.1% V-doped WSe2 confirms the existence of ferromagnetic order (Fig. 6b) [199].
To investigate the effect of magnetic-ion doping on changing the electronic structure and carrier-transport properties, field-effect
transistors (FETs) based on doped TMDs were fabricated [202,203]. Tang et al. found that low Nb-doped WS2 (2.5 at% Nb) exhibits
ambipolar conduction behaviour, while higher doping concentrations (4.7 at% Nb) induce p-type conduction, as evidenced by the I-V
curve shown in Fig. 6d [202]. Zhang et al. have demonstrated that the increase in carrier concentration tends to be offset by an
enhancement in the scattering by the charged impurities of the larger rhenium atoms doped in the MoS2 lattice [203]. Compared to
multilayer MoS2, which allows more physical conduction paths, carrier migration in single-layer MoS2 is more detrimental [203]. The
effect of doping of magnetic ions on photonic properties has also been discussed [24,203]. However, our purpose in forming 2D DMSs
is to generate local magnetic moments, improve magnetic coupling, and finally to achieve room-temperature ferromagnetism. V-doped
MoTe2 [205]/WSe2 [199]/WS2 [22] and Fe-doped MoS2 [24] have all been reported to possess room-temperature ferromagnetism.
M− H hysteresis loops are usually measured in experiments to determine the magnetic degradation temperature. The pronounced M− H
hysteresis loop at both cryogenic (5 K) and room temperatures, depicted in Fig. 6c, suggests that ferromagnetism is preserved up to
Fig. 6. Synthesis of semiconducting vanadium-doped monolayer WSe2 and ferromagnetic characteristics. (a) MFM phase images of pristine WSe2 at
room temperature. Scale bar, 10 μm. (b) Topography (left) and MFM (right) phase images of 0.1% vanadium-doped WSe2 at room temperature.
Scale bar, 10 μm. (c) Magnetization data of Fe: MoS2 monolayers at cryogenic and room temperatures, after subtracting the diamagnetic back
ground. A pronounced hysteresis loop is observed in Fe: MoS2 monolayers, suggesting ferromagnetism is preserved up to room temperature (300 K).
(d) Transport properties of the Nb-doped WS2. Transfer characteristics of FETs fabricated using pure WS2, 2.5 at% Nb-doped WS2, and 4.7 at% Nb-
doped WS2. Magnetization measurements of MoTe2 with different vanadium concentrations. (e) Variation in magnetization saturation with the
vanadium concentration. (f) Temperature dependences of HC and MS for the 0.8% vanadium-doped sample. The error bars reflect the experimental
uncertainty related to background noise. (g) Magnetization versus field loops at 300 K for pristine and vanadium-doped WS2 monolayers at 0.4, 2,
and 8 at% vanadium; scale bars are 2 nm. ((a) (b) reprinted with permission from Ref. [148] Copyright 2020 American Association for the
Advancement of Science; (c) Ref. [22] Copyright 2020 Nature Publishing Group; (d) Ref. [146] Copyright 2021 Wiley; (e) (f) Ref. [150] Copyright
2019 Wiley); (g) Ref. [20] Copyright 2020 Wiley).
16
room temperature in Fe-MoS2 [24]. Fig. 6e and f, demonstrating a weak decrease of Ms with increasing T in the accessible temperature
range, indicate a high value of Tc above room temperature in V-MoTe2 [205], which is significantly higher than the Tc ≈100 K reported
for MoTe2 promoted by intrinsic defects [206]. Fig. 6g presents smoothed M− H loops at 300 K of V-WS2, from which the Ms and Hc
values can be directly deduced, and the Tc is estimated to be about 470 K [22].
The experimental results and some calculations based on first principles [23,25,207,208] demonstrate that doping of magnetic ions
can indeed improve the magnetic-exchange interaction, thereby contributing to the realization of room-temperature 2D dilute mag
netic semiconductors, while the mechanism behind this is ambiguous as yet. According to the Mermin-Wagner theorem [9], no finite
ordering temperature in two dimensions will occur with isotropic Heisenberg exchange. However, TMD monolayers with the formula
MX2 do not have inversion symmetry, and SOC leads to a substantial splitting of the Kramers degenerate states at K and K’ with dxy/
dx2− y2 character [209]. SOC-induced level splitting of p-doped MoS2 results in a large single-ion magnetic anisotropy of about 5 meV in
the single impurity limit, and its magnetic-moment direction is preferentially perpendicular to the single-layer plane [210]. Analo
gously, in vanadium-doped WSe2 semiconductors, the localized V band is inverted at the valence-band edge by SOC, thereby leaving
spin-polarized hole carriers in the valence band. Consequently, the long-range ferromagnetic order is mediated with free holes to
establish the spin order, even near the W sites in the entire lattice [25]. A new interpretation, different from those proposed in the past,
is that the origin of the high Tc in Fe-doped GaSb and InSb bulk phases is not due to a carrier-induced mechanism but is attributed to the
concentration of impurities [23] which may be an inspiration for 2D DMSs, where concentration-dependent magnetic behaviour has
also been found [205]. The long-range magnetic mechanism of 2D DMSs is still unclear, the elucidation of which is the direction of
future efforts. Compared with conditional DMSs in bulk phases, a layer-dependency analysis may be the key point in 2DFMs [208].
The above-mentioned 2D ferromagnetic materials form with the involvement of elements, such as Cr, Fe, Mn and V with valence d-
electrons or f-electrons, in which the magnetic ordering originates from the partially filled d-bands or f-bands. The question that comes
to mind spontaneously is whether elements with only s/p-valence electrons could have high magnitudes of spin-wave stiffness caused
by spin splitting and magnetic order, leading to potentially higher Tc values. It has been demonstrated that carrier doping can
manipulate the long-range magnetic order and spin-polarization. Carrier doping can be realized by changing the total number of
electrons in the unit cell, with a compensating jellium background of opposite charge added [211]. Cao et al. first proposed the
possibility of carrier doping-induced tunable magnetism in quasi-2D semiconductors (GaSe) with tunable ferromagnetism and half-
metallicity [211]. For a range of hole-carrier densities, the averaged electron-spin magnetic moment of GaSe can be as large as
nearly 1.0 μB/carrier [211]. Our group predicted the new 2D semiconductor, InP3, whose robust ferromagnetic and half-metallic states
can be induced and tuned by p-type doping [14]. A semiconductor-to-metal transition was also revealed in the InP3 monolayer under
electron or high-concentration hole doping [14]. Yu et al. reported that hole doping can render CrI3 monolayers nearly 100% spin-
polarized at the Fermi level, enhancing the stability of itinerant ferromagnetism [212]. The origin of the carrier-doping-induced
tunable magnetism can be understood by considering the Stoner mechanism, according to the Stoner criterion ID(EF) greater than
1, where I is the Stoner parameter and D(EF) is the density of states at the Fermi energy [213]. Remarkable electrically tunable
magnetic ordering and MAE have been found in monolayers of CrSBr, where the magnetization easy axis can be tuned from being in-
plane to being out-of-plane by electrostatic doping [26]. The doping-induced tunability of MAE can be understood from a perturbation-
theory analysis, associated with a strong SOC effect of bromine, resulting in a larger impact of MAE for hole doping rather than for
electron doping [214].
5.1.2. Defect engineering

Defect engineering, which tunes the localized-defect electronic structures, can be another powerful strategy to regulate magnetism
[187,215]. Yang et al. systematically investigated the influence of point defects on monolayers of CrI3, including vacancies, interstitial,
substitution and bond-rotation defects [1]. The impacts of the vacancy defects on monolayer CrI3 are analogous to carrier doping,
where chromium or iodine vacancies induce p-type or n-type doping [207]. The FM-to-AFM transition in CrI3 is supposed to be
observed at a high defect concentration (~1.3 × 1013 cm− 2), originating from defect-induced local strain [207]. The defects can induce
local strain, further changing the Cr-Cr bond lengths with the distance from the defect. An antiferromagnetic state appeared when
LCr− Cr is less than 3.70 Å, while the ferromagnetic state was maintained when LCr− Cr is larger than 4.04 Å [207]. This indicates that the
defective state affects the local lattice structure and thus the magnetic exchange.
Sainbileg et al. considered two different oxygen defects, single O-attached or single O-doped structures, that significantly affect the
original structural architecture of the CrI3 monolayer [216]. Importantly, O-defective CrI3 monolayers possess robust exchange-
coupling parameters, suggesting a relatively higher Tc compared with the non-defective sheet without breaking the FM semi
conductor nature of CrI3 [216]. The enhanced exchange coupling originates from the disturbance of O-p states on Cr-d states, resulting
in a strong Jex and enhancement of Tc. Zhang et al. put forward an atomic engineering of the tungsten vacancy in monolayer WSe2 by
single potassium-atom decoration [217]. The potassium decoration alters the energy states and reshapes the wave function of the
defect states, which, therefore, leads to localized midgap states extending further into the vacuum. Interestingly, an unpaired electron
donated by the potassium atom can lead to a local magnetic moment, exhibiting an on–off switching by an odd–even number of
electron filling, suggesting the possibility of gate-programmable magnetic moments at the defects [217]. These studies demonstrate
that non-magnetic dopants could favour spontaneous spin polarization and local moment formation, as well as long-range magnetic
ordering.
5.1.3. Surface decoration

Modification of magnetic properties by adsorbing single atoms, functional groups and organic substances on the surface is a widely
used method to modulate the magnetism of 2D materials [151,218,219]. The modification of magnetic properties by surface
17
adsorption is mainly achieved by electron transfer and the generation of unpaired electrons. Such attempts were first implemented in
CrI3 and Cr2Ge2Te6 [10,11], which were first demonstrated to possess 2D ferromagnetism through experimental analyses. The
structures of H, O and Li atoms adsorbed on the CrI3 surface have been considered. Xu et al. found that the easy magnetization axis can
be tuned from being originally out-of-plane to being in the in-plane direction at certain coverages of Li [218]. The energy difference
between AFM and FM states and the Tc values are almost linearly enhanced as the Li coverage increases [218]. In Cr2Ge2Te6, both H
and alkali-metal adsorption surprisingly enhance the magnetic anisotropy energy by four times compared to that of pristine Cr2Ge2Te6,
leading to an increase of Tc by about 33% [21]. The redistribution of charge from H adatoms affects the neighbouring Te atoms,
altering the p-d hybridization between Cr-d and Te-P orbitals. Thus, this leads to the emergence of more localized Cr t2g spin-down
states and a change of magnetism with H adsorption on Cr2Ge2Te6 [21].
Due to the effect of the octahedral crystal field, the 3d electron orbitals of Cr are split into three t2g orbitals and two eg orbitals. In
pristine CrI3, each octahedrally coordinated Cr3+ ion has a 3d3 configuration, and the three t2g orbitals are singly occupied with
parallel spins. The adsorbed lithium atoms play a role similar to the introduction of donor impurities; the excess electrons occupy the
empty higher eg orbital according to Hund’s rules, resulting in a larger magnetic moment. When hydrogen atoms are adsorbed, one
spin-up electron transfers from the Cr-t2g state to a H-1s state, which results in a decrease of the total magnetic moment [218]. Of
course, the distortion of the crystal structure and crystal field due to the adsorbed atoms should also be considered. When an O atom is
exposed to the lower I atom in a CrI3 single-layer, it helps the I atom to break its bonds with the Cr atoms and completely destroys the
octahedral symmetry. The d states of Cr are no longer degenerate in two groups. The main hybridization is between the px/pz orbitals
of O and I atoms and one can see a very significant increase in Tc: Tc = 142 K compared with that of pristine CrI3 (Tc = 45 K) [20].
Fig. 7. (a) Schematic diagrams for orbital interactions, based on the tight-binding theorem, of monoclinic CrI3 bilayers. Red and blue bars represent
spin-up and -down states, respectively. (b) Optical micrograph of a tetralayer CrI3 tunnel-junction device. Electrons tunnel between two graphite
sheets separated by a magnetic CrI3 tunnel barrier. The entire stack is encapsulated in hexagonal boron nitride. (c) Schematic energy diagram of a
metal/ferromagnetic insulator/metal junction. The red and blue lines in the barrier region represent the spin-up and spin-down energy barriers,
respectively. (d) |d2I/dV2| (colour scale at right) versus applied magnetic field and DC bias voltage. All three inelastic peaks increase in energy as the
applied field is increased. (e) Four different magnetic configurations and spin-density distributions in the FGT monolayer, depicted as FM, AFM1,
AFM2, and AFM3 (upper panel). Energy difference between AFM3 and FM coupling and the total energy as a function of the applied strain in the
FGT monolayer (lower panel). (f) Side view of the atomic lattice of FGT (upper panel) and an optical-microscopy image of a typical FGT device on a
polyimide substrate (lower panel). The scale bar is 10 µm. (g) Schematic diagram of an FGT device in the strain experimental set-up. ((a) reprinted
with permission from Ref. [167] Copyright 2020 American Chemical Society; (b) (c) (d) Ref. [169] Copyright 2018 American Association for the
Advancement of Science; (e) Ref. [174] Copyright 2020 American Chemical Society. (f) (g) Ref. [186] Copyright 2020 Wiley). (For interpretation of
the references to colour in this figure legend, the reader is referred to the web version of this article.)
18
It is worth noting that different concentrations of single-atom adsorbates will also affect the MAE and magnetic moment. The MAE,
as well as Tc, of CrI3 shows a nearly linear relationship with the lithium adsorbate concentration [218]. The experimental reports
simultaneously found that when h-BN is fluorinated with different F concentrations, the corresponding values of magnetization and
band gap can also be changed [220]. The magnetization in fluorinated h-BN originates from the difference between up and down spin
states of the nitrogen atoms. At 6.25% F concentration, both up and down spin states are equivalent, leading to zero magnetization. As
the F concentration increases, the difference between the two spin states was enlarged, resulting in an enhanced net magnetization.
The reason is that the structure with 6.25% F concentration has two F atoms attached to B and nearest N atoms on opposite sides and
shows no magnetic moment due to the absence of unpaired electrons. Whereas for the configurations with 9.375, 12.5, and 15.625% F
concentrations, the asymmetric adsorption structures lead to different degrees of electron transfers, which in turn results in the
emergence of unpaired electrons, and thus a net magnetic moment. The corresponding values of magnetization are nearly equal to the
number of unpaired electrons present in the fluorinated h-BN sheet with different F concentrations [220]. These adsorption-
modification methods have also been applied to other two-dimensional ferromagnetic materials, such as the transition-metal halide
CrCl3, Graphdiyne, TMD monolayers and MXenes [18,19,221–223].
5.2. Inversion symmetry breaking
5.2.1. Electric field

Recent experimental findings of 2DFM behaviour in Fe3GeTe2, whose critical temperature can reach room temperature produced
by gating, has attracted great research interest [12]. The extraordinary properties of Fe3GeTe2 demonstrate that ionic-gating-induced
electron doping leads to manipulated magnetic properties, including Tc and an AFM-to-FM phase transition [224]. An interlayer phase
transition was also reported in CrI3 bilayers induced by an electric field alone, with the critical field being as low as 0.12 V/Å. The tight-
binding model shown in Fig. 7a proposed an explanation of the phase transition, whereby the orbital hopping, exchange splitting, and
crystal-field splitting cause EFM to drop more rapidly than EAFM as the electric field increases, leading to ΔE monotonically increasing
with the electric field [73]. Meanwhile, atomically thin CrI3 has been fabricated as dual-gate field-effect devices by controlling the
magnetism via a small gate voltage. An interlayer potential difference created by the external electric field leads to a linear magne
toelectric effect and interlayer spin-flip transitions [225]. The magnetism of tetralayer CrI3 insulators whose tunnel-junction device
depicted in Fig. 7b was detected by electron tunnelling [226]. A spin filter effect can be realized when electrons tunnel through a
ferromagnetic insulator as the spin-up and spin-down electrons have different barrier weights, as shown in Fig. 7c. The magnetic tunnel
barrier plays the role as an electric field to generate a “double spin filter” to employ in a magnetic memory bit [226]. Few-layered
Cr2Ge2Te6, mechanically exfoliated from a single crystal using the scotch-tape method, has been demonstrated to possess tunable
magnetism via gating, as characterized by micro-area Kerr measurements below Tc [227]. The tunable bipolar magnetism was
attributed to a realignment of the spin-polarized band structure with a shift in the Fermi level [227].
5.3. Rotational symmetry breaking
5.3.1. Strain engineering

Since precise doping and defect engineering in experiments is challenging, strain engineering as a mechanical-regulation method is
a promising route to modulate the electronic and magnetic properties of 2D materials without introducing defects [228–230].
Furthermore, strain engineering is suitable for 2D materials, as they can sustain much larger elastic strains than bulk materials [70].
A phase transition is a fascinating phenomenon observed in 2D materials when strain is applied. Graphene exhibits a phase
transition from a metallic to an insulating state by applying strain in different crystallographic directions [231,232]. The interesting
magnetic transition from AFM to FM states can also take place in half-fluorinated BN and GaN layers when applying strain, and a half-
metallic behaviour can be achieved at 6% compression [228,233]. Two-dimensional CrAsS4 is reported as having an AFM-to-FM
transition for a compressive strain of 1.76% along the one direction while there is a uniaxial tensile strain of 2.99% along the other
[234]. Doping and strain engineering combined can produce more intriguing phenomena: pristine monolayer VI3 displays an FM-to-
AFM phase transition with a robust semiconducting nature for 5% of compressive strain, while a fully-doped monolayer VI3 structure
exhibits an AFM-to-FM semiconducting transition at tensile strains larger than 4% [235]. Similar phase transitions have also been
reported in a wide range of other 2D materials, such as FeCl2 [236], CrTe3 [237], MoTeI [238] and MoS2 NRs [239]. Our group found
2D intrinsic ferromagnets from van der Waals antiferromagnets, which suggests a new direction to find high-Tc intrinsic ferromagnets.
We found that the single-layer 2D semiconductors, CrOX (CrOCl and CrOBr monolayers) show robust ferromagnetic ordering, large
spin polarization, and a high Tc (204 K under appropriate strains), and which can be easily exfoliated from their bulk antiferromagnetic
materials [13]. These 2D crystals promise great dynamical and thermal stabilities. The Tc of 2D CrOCl is 160 K, which exceeds the
record (155 K) of the most-studied dilute magnetic GaMnAs materials, and could be further enhanced by the application of appropriate
strains [13]. This achievement in 2D CrOCl led to the proposal to achieve a ferromagnetic monolayer by exfoliating the antiferro
magnetic bulk phase, which opens a new avenue for searching for 2D ferromagnetic materials [13]. Numerous researchers have re
ported that strain can control the anisotropy of MAE [19,240,241], which is essential for obtaining two-dimensional intrinsic
magnetism, according to the Mermin-Wagner theorem [9]. The MAE of chromium trihalides exhibits a strain dependence: it increases
when a compressive strain is applied in CrI3, while the opposite trend is observed in CrCl3 and CrBr3 [230]. In particular, the MAE of
CrI3 can be enhanced by 47% with a compressive strain of ε = 5% [230]. The Tc was also reported to be greatly boosted by strain, as in
CrSTe (from 295 K to 410 K with 5% strain) [97], and Cr2Ge2Se6 (from 144 K to 421 K with 5% strain) [242].
The stability of FM coupling can be understood using the GKA rules, which state that superexchange interactions are
19
antiferromagnetic in nature when the virtual electron transfer is between overlapping orbitals that are each half-filled, but they are
ferromagnetic when the virtual electron transfer is from a half-filled to an empty orbital or from a filled to a half-filled orbital [47–49].
Meanwhile, the GKA rule declares that the closer the bond angle is to 90 degrees, the stronger is the superexchange interaction
[47–49]. Considering that strain can change the bond length and the angle of bonds between atoms, combined with the GKA theorem,
it is not difficult to explain the controlling influence of strain on magnetism. It has been demonstrated that the ferromagnetism of FGT
can be largely enhanced by tensile strain (Fig. 7e), attributed to the competitive effects of direct exchange and superexchange in
teractions [228]. The direct exchange interaction gives rise to AFM coupling governed by the distance between the neighbouring Fe
atoms, while the superexchange interaction brings about FM coupling which is sensitive to the angle between Fe-Te/Ge-Fe bonds. The
competition between the direct exchange and superexchange interactions determines the magnetic ground state of FGT, which cor
responds to the phenomenon of a phase transition when applying strain. A similar situation has been confirmed and studied in CrSiTe3
[243], FeCl2 [236] and MoTeI [238]. Applying biaxial strains (compressive − 5% to tensile + 5%) to FeCl2 continuously changes the Fe-
Cl bond lengths of 1T-FeCl2 and maintains the Cl-Fe-Cl bond angle in the range of 90 ± 5 degrees. The Tc can also be greatly enhanced
from 13 K (pristine) to 82 K (zigzag-5% strain) [236]. In general, strain engineering alters the crystal lattice, such as the bond length
and bond angles, to modulate the magnetic coupling, according to the GKA theorem for superexchange interactions [47–49].
After the theoretical prediction, the magnetic regulation of FGT by strain was verified experimentally [12]. In order to apply tensile
strain to FGT, thin flakes of FGT (about 50 nm) were exfoliated directly onto a polyimide membrane and then were loaded into a
homemade strain setup with a three-point bending geometry, as shown schematically in Fig. 7f and g [229]. Uniaxial tensile strain can
be achieved by pushing the needle to the centre of the substrate. The value of Tc, measured by a field-cooled measurement, exhibits an
increase from 180 to 210 K as the strain is enhanced from 0% to 0.65%. Meanwhile, the coercive field Hc exhibits a remarkable
enhancement under strain. It is noteworthy that the process of magnetization reversal is achieved with the magnetic field kept at 0.2 T.
The strain dependence of magnetic parameters, such as Hc and Tc in FGT, was attributed to the variation of MAE which is mainly
determined by the SOC [244] by an analysis using density-functional methods. The results indicate that the SOC strengthens with
respect to the crystal-lattice expansion under tensile strain, verified by the enlarged orbital portion of the magnetic moment under
strain [229]. This suggests again that MAE plays a key role in maintaining long-range magnetic order and thus significantly increases
the Tc by suppressing thermal fluctuations.
Fig. 8. (a) Schematic diagrams of orbital evolution and the origin of energy-level staggering in Cr, W alloy systems. Red and cyan bars represent
spin-up and spin-down orbitals, respectively. uCr and uW are exchange splittings for Cr- and W-d orbitals, respectively. Δc is the energy gap opened
up by the crystal field. (b) Cluster model, crystal field and superexchange path with atomic-orbital-based schematic diagrams of octahedral (left
panel) and tetrahedral (right panel) models. (c) The pure phase and one of the typical alloy phases for CrI3-or CrGeTe3-based systems. (d) Magnetic
moment per site as a function of temperature for CrI3, CrWI6 monolayer, and CrWGe2Te6 monolayer under 4% tensile strain from Monte Carlo
simulations. (e) SEM micrographs and EDX of undoped (left panel) and Gd-doped (right panel) Ti3C2Tx MXene. ((a) (c) (d) reprinted with permission
from Ref. [188] Copyright 2018 American Chemical Society; (b) Ref. [190] Copyright 2019 American Chemical Society; (e) Ref. [197] Copyright
2020 Elsevier). (For interpretation of the references to colour in this figure legend, the reader is referred to the web version of this article.)
20
Fig. 9. (a) Representation of topological charge (top) of the skyrmion (bottom). (b) Triangular skyrmion lattice (c) Upper panel: schematic of the
magnetization in both the ferromagnetic and antiferromagnetic layers during the illumination process. Lower panel: calculated z-component of the
effective field during the illumination (before the skyrmion creation happens). The red circle is the X-ray illumination region. The yellow arrows
schematically indicate the influence of the effective field. (d) The schematic energy landscape of the ferromagnetic state and skyrmion state before,
during, and after the X-ray illumination. The energies were calculated via micromagnetic simulations. (e) Schematic diagram of a Néel-type sky
rmion on a tilted sample for LTEM imaging. The orange and blue circles are for positive and negative magnetizations along the z direction,
respectively. Brown arrows indicate the in-plane magnetization component, while grey arrows indicate the Lorentz force. (f) LTEM observation of a
skyrmion lattice from under-focus to over-focus for WTe2/40L Fe3GeTe2 samples. ((a) reprinted with permission from Ref. [199] Copyright 2020
American Chemical Society; (b) (c) (d) Ref. [204] Copyright 2020 Nature Publishing Group; (e) (f) Ref. [198]). (For interpretation of the references
to colour in this figure legend, the reader is referred to the web version of this article.)
21
5.4. Alloying and rare-earth atom doping
In addition to traditional control methods, the Tc has recently been improved and understood from the perspectives of orbital
adjustment, alloying and formation of rare-metal systems, opening up a new way to modulate the 2D magnetism. Huang et al. pointed
out that the weakness of ferromagnetism in CrI3 is due to the large Gex between half-occupied t2g↑ and empty eg↑ orbitals by analysing a
double-orbital model from the perspective of the tight-binding theorem [188]. EFM shows a positive correlation with Gex, while EAFM is
independent of Gex, indicating that Eex (=EAFM − EFM) can be enhanced as Gex decreases. An isovalent-alloying method was proposed to
reduce the energy gap and increase the virtual exchange between t2g↑ and eg↑ orbitals [188]. Since tungsten (W) exhibits the same
valence state (+3) and occupation state (d3) as Cr, and has a much smaller exchange splitting than Cr, W was chosen for alloying CrI3
and CrGeTe3. Schematic diagrams of Gex and W alloying are shown in Fig. 8a and c. Alloyed CrI3 and CrGeTe3 indeed show a significant
increase of Tc from CrI3, as depicted in Fig. 8d [188]. The isovalent-alloying method to increase ferromagnetic exchange was also
adopted for MnS2 where a large enhancement of Tc was observed in Mn2ReS6 [245]. Huang et al. found high-Tc intrinsic FM semi
conductors in a tetrahedrally coordinated system different from those containing octahedrally coordinated magnetic ions, such as
CrBr3, EuO, CdCr2S4 spinel, and BiMnO3 perovskite. FM couplings in the tetrahedral crystal are inherently stronger, since Eex for the
tetrahedral crystal is larger than that for the octahedral crystal, as demonstrated in Fig. 8b [246].
Rare-earth elements have rarely been investigated for high-Tc 2D FMSs as the exchange interaction mediated by anions is usually
very weak, owing to the highly localized characteristic of 4f electrons. Gadolinium is the most attractive heavy rare-earth metal
[247,248] having a half-filled and well-localized 4f subshell, leading to ferromagnetic behaviour with a high saturation magnetization
[249]. Wang et al. first demonstrated the feasibility of realizing promising high-Tc FMS in 2D rare-earth halides (GdI2 monolayer)
[250]. Considerable Gd 4f-Gd 5d interactions within each Gd2+ ion, together with significant Gd 5d-(I 5p)-Gd 5d interactions, lead to
strong ferromagnetism in the 2D limit, i.e. a high Tc (~241 K) [250]. Gd2B2 was subsequently demonstrated to possess a ferromagnetic
ground state with a high permanent magnetic moment far above room temperature [251]. The 1T GdN2 monolayer was reported to be
a promising p-state magnetic Dirac semiconductor with a high Tc and large MAE by theoretical analysis. A gap of N 2p Dirac bands
opened by SOC was found in 1T GdN2 monolayers, together with a band shift induced by exchange in the Gd 4f7 half-full shell [252].
Apart from the intrinsic 2D Gd-based monolayer, 2D Gd-doped systems are also appealing for room-temperature ferromagnetism
research [150]. A high magnetic moment at room temperature, with a stable ferromagnetic hysteresis loop, was demonstrated in a Gd-
doped sample of Ti3C2Tx (Fig. 8e), which originated from the enhanced spin density of Ti-3d states around the Fermi level after Gd
doping [150].
6. Intriguing physical phenomena for electronic devices
Internal magnetic order can simultaneously exhibit other physical characteristics, like specific topological features which bring out
some intriguing properties, such as skyrmions [253] and QAHE [110]. Meanwhile, spins interplaying with charges or photons leads to
unique effects, for instance multiferroics [254] and magneto-optics, [255] which can be applied for electronics devices. Hereafter, we
introduce these exceptional properties in 2D magnetic materials to explore the principles and applications.
6.1. Skyrmions
Skyrmions are localized solitonic spin textures with protected topology, which are promising as information carriers in ultra-dense,
energy-efficient logic and memory devices [256,257]. To create magnetic skyrmions, surface acoustic waves (SAWs) were employed in
asymmetric multilayers of Pt/Co/Ir [258]. The propagating SAWs induce skyrmions in a wide area of the magnetic film. The skyrmion
schematic diagram and triangular skyrmion lattice are shown in Fig. 9a [259] and b [260]. In ultrathin magnetic films, skyrmions were
observed in Fe monolayers and in PdFe bilayers grown on Ir (1 1 1) surfaces at the Fe/Ir interface [261]. Nevertheless, the necessity of
having large magnetic fields (over 1 T) and low temperatures for stabilization of the skyrmions has hindered the development of
memory devices, which therefore encourages the exploration of the use of skyrmions in low-dimensional magnetic materials. Dzya
loshinskii–Moriya interactions (DMIs), induced by Rashba spin–orbit coupling in the absence of inversion symmetry, [262] give rise to
the emergence of skyrmions. However, most of the currently known van der Waals ferromagnetic materials have inversion-symmetry
properties, which brings about no DMIs, such as CrI3 and Cr2Ge2Te6.
The Curie transition temperature of 2D FGT is about 230 K and can be adjusted above room temperature by Ga implantation [263].
Previous studies have shown that the FGT material is etched into a rhombus structure by focused ion-beam etching technology. The
magnetic domain structure of FGT is transformed from an out-of-plane magnetic domain structure at low temperature to a high-
temperature in-plane vortex magnetic domain structure [264]. This unique property makes FGT an ideal platform for constructing
magnetic skyrmions. However, the skyrmions in van der Waals materials are almost always induced by the magnetic field at an
external interface, except for some theoretical results. This leads to a discussion of the physical mechanism of skyrmions under a
magnetic field: namely, whether the formation of skyrmions is due to the intrinsic properties of the material or the induction of
external magnetic fields. Yang et al. have demonstrated the existence of skyrmions in the van der Waals ferromagnet FGT on a (Co/Pd)n
superlattice without an external magnetic field, which provides an effective method to induce magnetic skyrmions in vdW magnets at
zero magnetic field in magnetic heterostructures [265]. Simultaneously, a method to create individual skyrmions at zero-field in an
exchange-biased magnetic multilayer on exposure to soft X-rays was proposed [260]. The X-rays will have an impact on the anti
ferromagnetic order and the corresponding exchange bias, shown in Fig. 9c and d, leading to the creation and modulation of single
skyrmions [260].
22
Several ways have been proposed to break the inversion symmetry in 2D systems for intrinsic DMI and skyrmions, such as an
electric field [266], Moiré rotation [267] and heterostructures [268]. In 2D CrI3, the impact of the electric field on the DMIs has been
reported [266] and the existence of skyrmions was observed by combining density-functional theory and atomistic spin-dynamics
simulations [269]. The magneto-crystalline anisotropy and DMIs induced by a vertical electric field of 2 V/nm breaks the inversion
symmetry, which facilitates the hosting of skyrmions with a diameter less than 10 nm at 0 K [269]. DMIs and Néel-type skyrmions were
demonstrated in WTe2/FGT van der Waals heterostructures and the topological Hall effect was determined from Lorentz transmission
electron microscopy (Fig. 9e and f). The sizes of the directly observed skyrmions were ~ 150 nm at 94 K and ~ 80 nm at 198 K [253].
The mechanism of the formation of skyrmions in WTe2/FGT van der Waals heterostructures originates from the interplay between the
exchange interaction, magnetic anisotropy and the dipolar interaction. The reduced thickness of FGT flakes decreases the dipolar
interaction, and thus, perpendicular magnetic anisotropy leads to a stabilized single domain [253]. Monolayer Janus MnSTe, MnSeTe,
Fig. 10. (a) Anomalous Hall conductivity of PdBr3 monolayers as a function of energy near the Fermi level. (b) The surface states of PdBr3
monolayers. (c) Diagram of a multi-terminal Hall bar graphene/Fe-SnS2 hybrid device. (d) The transfer curve of longitudinal resistance. Inset:
optical image of the graphene/Fe-SnS2 hybrid device. The Fe-SnS2 nanoplate is placed on Hall-bar shaped graphene. (e) Data-driven discovery
pipeline for vdW heterojunction-based QAH systems. ((a) (b) reprinted with permission from Ref. [229] Copyright 2019 American Physical Society;
(c) (d) Ref. [234] Copyright 2021 American Physical Society; (e) Ref. [238] Copyright 2020 Nature Publishing Group).
23
and VSeTe have significant intrinsic DMIs originating from the Te atoms in the case of out-of-plane geometric asymmetry and strong
SOC, which could stabilize the sub-50 nm intrinsic skyrmions in monolayer MnSTe and MnSeTe at zero magnetic field [270]. Stable
Bloch-type skyrmion bubble lattices were observed in FGT [271] and Cr2Ge2Te6 [272], which are critical for the exploitation of 2D
vdW skyrmion-based devices.
6.2. Quantum anomalous Hall effect
Internal magnetic order with nontrivial topology in 2D materials can induce the QAHE, which is essentially due to the breaking of
time-reversal symmetry. This is inspired by the seminal work of Haldane with a honeycomb lattice structure [273]. The quantized Hall
effect is generated without a strong external magnetic field, where ferromagnetic ordering and strong SOC engender a band gap in the
Fig. 11. (a) Schematic drawing of possible magnetoelectric couplings. Left: a charge dipole, indicative of ferroelectricity. Right: a magnetic
moment, indicative of magnetism. Three ‘glues’ are shown that can link these two vectors. (b) Magnetoelectric effect in In2Se3, mediated by the
magnetic proximity to Cr2Ge2Te6. Interlayer-distance dependence of the proximity-induced Se1 and In1 spin moments. (c) Multistate control of two-
dimensional multiferroic bilayer VS2. The red and grey arrows represent the spin directions of the bottom layer and top layer of VS2, respectively.
The blue arrows represent the ferroelectric polarization direction of the system. (d) Total magnetic moments (without SOC) on bilayer VS2 as a
function of the interlayer-distance variation and external electric field. (e) Variation of spontaneous electric polarization and ground-state magnetic
ordering in the VOCl2 monolayer with in-plane biaxial tensile strain. (f) The schematic procedure for discovering ferroelectric materials, MIMIIP2X6.
((a) reprinted with permission from Ref. [242] Copyright 2019 Science China Press; (b) Ref. [246] Copyright 2019 Nature Publishing Group; (c) (d)
Ref. [252] Copyright 2020 American Physical Society; (e) Ref. [254] Copyright 2021 American Physical Society; (f) Ref. [257] Copyright 2021
Elsevier). (For interpretation of the references to colour in this figure legend, the reader is referred to the web version of this article.)
24
bulk and gapless chiral edge states at boundaries [273–277]. The dissipationless metallic chiral edge states with quantized conduc
tivity enable QAHE, which is appealing for high-efficiency quantum devices and spintronic applications [278,279]. Two conditions
must be satisfied for QAHE in 2D materials: broken time-reversal symmetry with a certain magnetic ordering, and a non-zero Chern
number for the occupied bands. The establishment of FM order in 2D materials will introduce exchange splitting, which could destroy
the band-inversion symmetry and bring about the QAHE.
Quantization of the Hall resistance at a value of h/e2 at 30 mK in Cr-doped (Bi, Sb)2Te3 films without an external magnetic field was
first observed by Chang et al [280]. Nevertheless, the ultra-low temperature (less than 100 mK) of QAHE reported in the experiments
on Cr- or V-doped (Bi,Sb)2Te3 [280,281] films calls for a quantum anomalous Hall insulator with a large band gap, high Tc and,
simultaneously, a high carrier mobility. Several 2D transition-metal tri-halides were predicted to exhibit the QAHE, such as RuI3 [282],
ReX3 [283] (X = Br, I), and MnX3 [284] (X = F, Cl, Br, I). 14 transition-metal tri-bromide monolayers were recently investigated by
theoretical methods, among which VBr3, FeBr3, NiBr3, and PdBr3 are endowed with intrinsic half-metallicity and possess quantum
anomalous Hall insulating phases [15]. The theoretical Tc values are ~ 190, 100 and 110 K for VBr3, NiBr3 and PdBr3, [15] respec
tively, which are significantly improved compared to the experimental observations. The band structures with SOC and surface states
are shown in Fig. 10a and b and demonstrate the existence of QAHE states [285]. 2D V2O3 is notable with an unexceptional ferro
magnetic Tc (about 900 K) and a non-zero Chern number. The large band gap in V2O3 is induced by a cooperative effect of electron
correlation and SOC together, instead of a large SOC magnitude itself [286]. 2D FeX3 (X = Cl, Br, I) were predicted as intrinsic Dirac
half-metals with quantized Hall conductivity, gapless chiral edge states and relatively high Tc (116–175 K). A quantum phase transition
of monolayer FeX3 from a QAH insulator to a metal and finally to a trivial Mott insulator was observed when the Hubbard U was
moderately increased [287,288].
Exploring vdW heterostructures with FM orders driven by proximity effects is another effective way to enhance the working
temperature of QAHE. Graphene is a unique 2D monolayer material with a honeycomb lattice formed by carbon atoms. It has become
an ideal prototype material for engineering the QAHE according to the Haldane model [273]. Graphene-based heterostructures have
been widely investigated, such as graphene/CrI3 [111], graphene/CrBr3 [112], graphene/NiI2 [110] and graphene/FexSn1− xS2 [289]
heterostructures. A diagram of a multi-terminal Hall bar graphene/Fe-SnS2 hybrid device and the transfer curve of longitudinal
resistance are depicted in Fig. 10c and d. The breakthrough in experiments on graphene/Fe-SnS2 has led to a huge exploration of its
applications in electronic devices [289]. The perpendicular magnetic anisotropy of graphene/NiI2 heterostructures can be effectively
enhanced owing to the graphene proximity and the competition between py, px hybridization and py, pz hybridization of Iodine atoms,
which in turn enhances the intrinsic magnetic order [110]. The enhancement of the magnetic-proximity effect on interlayer exchange
coupling and nontrivial band gaps was further observed in vdW heterostructures for QAHE, such as germanene/Cr2Ge2Te6 [290],
Bi2− xSbxTe3− ySey/Cr2Ge2Te6 [291] and MnBi2Te4/CrI3 [292].
Data-driven methods to accelerate the discovery of 2D magnetic materials with QAHE is the new way to follow. A computational
screening of topological two-dimensional materials from the Computational 2D Materials Database (C2DB) database [293] was
employed, and a total of 48 quantum spin Hall insulators, seven quantum anomalous Hall insulators, and 21 crystalline topological
insulators were found [294]. A high-throughput filtering was proposed for heterojunction-based 2D magnetic topological systems that
host the QAHE by combining data-driven materials search, first-principles calculations, and symmetry-based analytical models, as
illustrated in Fig. 10e. 46 potential magnetic semiconductors were screened out and the MnNF/MnNCl heterojunction with FM was
demonstrated to possess the QAHE stacking by combining first-principles calculations and a symmetry analysis [295]. Especially for
MXenes, valley-Polarized Quantum Anomalous Hall Effect (VP-QAH) in MXenes led to in-depth research, by a high-throughput first-
principles approach, and 14 MXenes were identified with nonzero bulk Chern numbers [296]. At present, high-throughput screening
has greatly accelerated the speed of material discovery, while there is still relatively little research of machine learning on the physical
properties of these material data, which is an urgent need to overcome.
6.3. Magnetoelectricity
Magnetism and electricity are two fundamental physical phenomena originating from the spin and the charge degrees of freedom,
respectively [297]. An emergent branch of condensed-matter physics, called magnetoelectricity, has been developed with a crossover
between these two fascinating topics (Fig. 11a) [298–301]. The magnetic moments are generated by unpaired electrons in partially
occupied d orbitals and/or f orbitals, while the spontaneous formation of a charge dipole usually needs empty d orbitals, which is
called the d0 rule [302]. The incompatibility of magnetism and electricity conceptually determines the challenges for realizing
magnetoelectricity.
The roles of ferromagnetic materials in the application of magnetoelectricity includes two factors. One is combining two separate
materials with ferroelectricity and ferromagnetism to circumvent the deadlock and prompts the flourishing of explorations for mul
tiferroic heterostructures. Intriguing physical phenomena and strong magnetoelectric-coupling mechanisms may develop at the
complex interface in the heterostructures. When the direction of the ferroelectric (FE) polarization is reversed, a transition from FM to
AFM coupling of FeI2 and bilayer CrI3 was observed in 2D In2Se3/FeI2 [303] and Sc2CO2/bilayer CrI3 [304] heterostructures,
respectively. Meanwhile, the MAE of Cr2Ge2Te6 can change between the easy-axis and easy-plane in 2D In2Se3/Cr2Ge2Te6, hinging on
the polarization direction of In2Se3 [305]. Carrier doping, as well as an external vertical electric field, can also be applied to control the
magnetic states by switching the electric polarization of FE, which has been demonstrated in 2D CuInP2S6/InSe [306] and transition
metal phthalocyanine (TMPc)/In2Se3 [307] van der Waals heterostructures, respectively. The controlling behaviour of the substrate
for ferroelectricity in SnTe originates from the electronic level. For instance, enhancing ferroelectric polarization and inducing
magnetism were observed in SnTe/MgO (0 0 1) heterostructures [308].
25
Another factor is the realization of strong magnetic-electric coupling in 2D ferromagnetic materials. Monolayers of the VOX2 (X =
Cl, Br, I) family, as single-phase one-cation multiferroics, have been determined to violate the d0 rule. The partially occupied d-orbital
of VOX2 (X = Cl, Br, I) lies in a plane perpendicular to the ferroelectric polarization, enhancing the electric polarization in these
monolayers [309,310]. Ferroelectricity and AFM coupling by a ferrovalley were found in bilayer VS2 multiferroic material [311].
Surprisingly, arbitrary switching in all four different ferroelectric antiferromagnetic configurations of VS2 can be realized using an
external magnetic field and electric field (Fig. 11c), raising great possibilities for realizing multistate storage. Furthermore, giant linear
and second-order nonlinear magnetoelectric coupling can be achieved by manipulating the interlayer distance, [311] as demonstrated
in Fig. 11b and d. The coexistence of three ferroic scenarios, FE, AFM and ferroelastic states, was strictly demonstrated as well in
hydroxyl-oxidized iron (FeOOH) monolayers [312]. The AFM ordering in the FeOOH monolayer originates from the superexchange
interaction. The Fe–O–Fe bond angle along the [99] direction is 152.91 degrees, suggesting strong antiferromagnetic coupling along
this direction, according to the GKA rules [47–49].
Some peculiar modification techniques, including strain, doping and electrical control, have been adopted to multiferroics.
Magnetic-ordering and electric polarization of 2D AFM-FE VOCl2 monolayers can be tuned independently by applying uniaxial tensile
Fig. 12. (a) Schematic illustration of magneto-optical Kerr and Faraday effects in two-dimensional ferromagnetic materials. (b) Schematic of the
polar Kerr effect. Schematic of the metamaterial structure. It consists of a normal magneto-optical material, such as bismuth iron garnet (blue layer)
←̅̅̅
̅̅̅̅→
̅
and a metal (yellow layer). χ m and χ are polarizabilities of the metal and magneto-optical material, respectively. (c) The calculated |V| as a
function of the filling ratio fm when χ d = 5:25 and χ 0 = 0:06272. (d) Kerr rotation (θK) and ellipticity (εK) spectra of: a) bulk; b) monolayer; c)
bilayer; and d) trilayer CrI3. The filled red circle in each panel indicates the θK value from the recent experiment. (e) Schematic illustration of the
enhancement of magneto-optical effects in a nanoscale structure. Linearly polarized light is focused on a dielectric metasurface composed of silicon
nanoparticles supporting magnetic Mie-type resonances, the metasurface being covered by a thin nickel film. The sample is subjected to the action of
an external magnetic field oriented perpendicular to the wave vector of the incident light. The inset shows an SEM image of the sample. ((a) (d)
reprinted with permission from Ref. [258] Copyright 2019 Institute of Physics Publishing; (b) (c) Ref. [267] Copyright 2020 American Physical
Society; (e) Ref. [270] Copyright 2017 American Chemical Society). (For interpretation of the references to colour in this figure legend, the reader is
referred to the web version of this article.)
26
strain along different in-plane lattice vectors, as depicted in Fig. 11e. A phase transition from the AFM ground state with an out-of-
plane magnetization to a FM ground state with an in-plane magnetization can be obtained when applying 4% tensile strain [313].
Two kinds of exchange interactions among V ions were considered to explain the phase transition in VOCl2. Direct exchange in
teractions dominate up to 3% tensile strain and superexchange interactions takes control for tensile strains of 4% and above. Therefore,
the degree of localization of electrons is different for different strain states and the magnetic coupling mechanism needs to be carefully
considered. The coexistence of FE and FM in two-dimensional Fe-doped In2Se3 (Fe0.16In1.84Se3) was predicted in a theoretical
approach, which was further experimentally confirmed by magnetic measurements [314]. The AFM-to-FM phase transition can be
realized by reversing the in-plane electric polarization through the application of an external electric field in a single-phase 2D
multiferroic ReWCl6 monolayer [315].
High-throughput ab initio calculations and data-driven machine-learning schemes with a set of new electronic orbital-based de
scriptors were exploited to discern 60 novel and stable ferroelectric materials out of 2964 structures, including 16 ferroelectric metals
and 44 ferroelectric semiconductors [316]. The workflow is shown in Fig. 11f. Furthermore, a machine-learning method to search for
geometric patterns of magnetoelectric multi-phase composites has been proposed, utilizing both the convolution neural network
(CNN) and artificial neural network (ANN) algorithms [317]. A two-dimensional finite element method was adopted to calculate the
magnetoelectric coupling coefficients, which were utilized to establish the database, as the input data for ML-based optimization
[317]. The coupling effect and ranked optical patterns can be accurately predicted with limited data by this ML method. Combining
high-throughput screening and machine learning is the future direction for developing 2D multiferroics, and is certain to accelerate the
exploration of high-performance magnetoelectric materials.
6.4. Magneto-optical effect
The magneto-optical effects (MOEs) refer to the change of the polarization state of light when interacting with magnetic materials
[318]. When a linearly polarized light beam hits a magnetic material, the reflected and transmitted light beams become elliptically
polarized, with the principal axis rotated with respect to the polarization direction of the incident light beam, as illustrated in Fig. 12a
[319]. The MOKE and magneto-optical Faraday effects (MOFE) are shown in Fig. 12a as well [320]. Magnetic materials with large
MOKE effects would find valuable MO storage and sensor applications, and hence have been continuously researched for decades.
Researchers have investigated MO effects in monolayers, bilayers and trilayers, as well as bulk, of Fe3GeTe2 [321], Cr2Ge2Te6 [322]
and CrI3 [319]. The calculated magneto-optical spectra show large magnetic circular dichroism, thus resulting in large MO Kerr
rotation and Faraday rotation angles. Throughout all structures of Fe3GeTe2, Cr2Ge2Te6 and CrI3, the MO Kerr rotation spectra are
similar, due to the weak interlayer coupling. Generally, the Kerr rotation spectrum starts with a negative peak but becomes large and
oscillatory with an increase of photon energy. The maximum value of the positive Kerr rotation angle of all structures appears at
approximately the same interval. The complex MO Faraday rotation has also been calculated for 1–3 layers and the bulk, with the
results being shown in Fig. 12d. The MO Faraday rotation spectra are similar to that of the MO Kerr rotation spectra in all considered
structures. MOEs are a powerful probe of magnetism in 2D materials. These findings of such single-spin ferromagnetic semiconducting
thin films suggest that they will find valuable applications in semiconductor MO and spintronic nanodevices.
Non-reciprocal optics has important applications in optical isolators and circulators [323] and is also used to explore intriguing
topological properties of light, such as the optical analogue of the quantum Hall effect [324]. These devices and optical phenomena
rely on breaking the time-reversal symmetry to realize non-reciprocal responses. MOE is the most effective way to break the time-
reversal symmetry [325,326]. Unfortunately, the MOE is extremely weak at optical frequencies due to the intrinsic limit of natural
materials [327]. Researchers have shown that magneto-optical metamaterials which combine normal magneto-optical materials, such
as bismuth iron garnet (blue layer) and a metal (yellow layer) (Fig. 12b) could exhibit a greatly enhanced magneto-optical effect [328].
In contrast to the common way to enhance the magneto-optical effect through optical resonance, the enhancement is realized by
directly engineering the effective dielectric tensor of the metamaterials (Fig. 12c) [329,330]. In addition, researchers have extended
the concept of high-index resonant nanophotonics to the case of magnetically active materials and have studied the MO response of a
dielectric metasurface covered with a thin magnetic film to enhance the MOE, as shown schematically in Fig. 12e. A nanoantenna is a
resonant element that supports both electric and magnetic multipolar modes that can be excited efficiently for optical magnetism
effects. It was demonstrated that the optical magnetism associated with the magnetic dipole Mie resonance in a single silicon nanodisk
leads to a manyfold enhancement of the magneto-optical response of the hybrid magnetophotonic metasurface in comparison with a
thin nickel film deposited on a flat silica substrate [331].
MOE can be regulated by doping holes in two-dimensional materials, including metal-monochalcogenide monolayers [332], blue
phosphorene, grey arsenene [333] and nitrogen–graphene crystals [334] with a ferromagnetic ground state. Ferromagnetic ground
states are found in them due to a Stoner electronic instability, which originates from the van Hove singularity of the density of states at
the valence-band edge. Doping concentrations are electrically controllable by adjusting the number of holes via the gate voltage. Kerr
and Faraday rotation angles first become larger with increasing hole concentration until reaching their maximum values, and then
diminish for larger hole concentrations due to the recovery of the non-magnetic state [332]. The large MOEs are attributed to the large
off-diagonal components of the optical conductivity. In short, the strength of the magneto-optical effect can be controlled by
manipulating the doping concentration. The superior MO characteristics of these materials make them an exciting platform for the
development of multifunctional information-storage devices.
27
7. Opportunities and challenges
In the previous sections, progress for 2D magnetic materials was introduced, including the physical theories, peculiar properties
and applications. The science of thin-layer magnetism has attracted worldwide attention and could ultimately lead to truly trans
formative technologies, including dramatically changing the landscape of data storage, information processing, and spintronics [335].
However, identifying the challenges to pursue and problems to solve are critical for the rapid development of 2D magnetic materials. In
the following section, we have summarized some of the challenges and future prospects of 2D magnetic materials.
7.1. Fundamental theory
7.1.1. Mermin-Wagner theorem

The Mermin–Wagner theorem states that thermal fluctuations prevent long-range order, breaking continuous symmetries in low-
dimensional systems for the isotropic Heisenberg model at finite temperatures [9]. Therefore, the Mermin–Wagner theorem has been
regarded as a milestone for decades, driving the research of low-dimensional magnetic materials, that is, the search for materials with
large magnetic anisotropy to resist thermal perturbations [322,336]. However it has been realized that the theorem becomes physi
cally effective only for astronomical sample sizes, and therefore 2D magnets at finite temperature in practical sizes could be achieved
[337]. It was proposed that finite-size effects, disorder and exchange coupling can be utilized to maintain the stabilized magnetic order
at finite temperatures without large-enough magnetic anisotropy for practical implementations [337]. Studying the effect of finite-size
effects on magnetic order through spin-dynamics simulations is crucial to guide experimental synthesis, as well as theoretical
breakthroughs, in the near future.
7.1.2. Curie temperature

The Curie temperatures of 2D vdW magnets observed in experiments are much lower than room temperature, in contrast to the high
Curie temperatures predicted by the theoretical calculations [10,11]. The core reason is that these predicted materials with high Curie
temperatures are difficult to prepare, for example Mn2NT2 (T = F, O, OH), whose Tc values are reported as 1877 K, 1379 K, 1745 K
respectively. Furthermore, even theoretical predictions can sometimes vary widely between models. Table 2 lists some of the dif
ferences in the magnetic ground state and predicted Curie temperatures due to model choice and Hubbard U-value differences. In view
of the above two situations, first, we can screen out more stable, easy-to-synthesize, and high-transition-temperature 2D magnetic
materials through high-throughput computing, providing more choices for experimental synthesis. Based on the filtered data, com
bined with machine learning, new materials can be predicted with high Curie temperatures. Secondly, it is necessary to carefully deal
with the U value and pay attention to the selection of the model in theoretical calculations.
7.2. Synthesis and stability
Currently, two-dimensional magnetic materials are prepared by various methods, including mechanical exfoliation [338,339],
chemical vapor deposition (CVD) [68,340], liquid exfoliation [341,342] and molecular beam epitaxy [81,343]. Among them, me
chanical exfoliation and molecular beam epitaxy are the mainstream methods for preparing two-dimensional materials. Although the
two-dimensional materials prepared by the mechanical exfoliation method have many advantages, such as fewer defects and smooth
surfaces [344], this method has disadvantages such as low production efficiency and poor controllability, which makes it difficult to
Table 2
Magnetic ground states and Curie temperatures with the choice of Hubbard U and magnetic models.
Compositions U (eV) GS Model Tc
Cr2B2 4.0 FM – –
3.0 FM – –
0.0 AFM – –
Fe2B2 0.0 FM – –
GGA & HSE AFM – –
NiCl2 2.0 FM Heisenberg 57 [174]
4.0 FM Heisenberg 205 [376]
MnBr3 3.9 FM Heisenberg 810 [284]
MnI3 3.9 FM Heisenberg 820 [284]
VI3 3.0 FM Heisenberg 27 [379]
GdI2 9.2 FM Heisenberg 241 [250]
9.2 FM Ising 745 [250]
CrI3 – FM Experiment 45 [10]
1.0 FM Mean field theory 109 [381]
2.65 FM Ising 107 [382]
– FM Heisenberg 46 [383]
28
achieve large-scale synthesis and industrialized mass production [345].

Compared to mechanical exfoliation, molecular beam epitaxy (MBE) can realize wafer-size scalability, crystallinity and atomically
precise thickness controls, and the epitaxial growth of MoSe2 thin films on mica can be achieved by the MBE method [346]. MBE has
been widely utilized as a powerful tool for rapid expansion of TMDs, among which some are 2D vdW magnets [346]. Nevertheless, the
controlled monolayer growth of 2D magnets is the major challenge, which requires a deep consideration of substrate-induced effects.
CVD techniques, whose chemical reactions can be controlled by gas chemistry [347], benefits the high-quality synthesis of many 2D
materials, such as graphene [348], h-BN [349] and TMDs [350]. Developing CVD methods to improve the quality of magnetic 2D
materials is one of the important directions for the future progress of magnetic 2D materials.
Until recently, the synthesis of atomically thin, large-area 2D magnetic layers faced many challenges, including the stability of the
synthesized 2D magnets. Most synthesized 2D magnetic materials are very sensitive to oxygenation, moisture and temperatures [351].
In the laboratory, we can transfer samples directly to a glove box without interacting with air or applying a protective layer in situ,
which is impossible in practical applications. Therefore, it is critical to find and synthesize more air-stable 2D magnets [352] or
improve the stability of magnetic materials through coating [353] or other means in the near future. Apart from the stability, some
other challenges exist as well for large-scale 2D magnetic layers. As functional groups are widely applied to modulate the magnetic
properties of 2D magnets [76] and to form Janus structures [354], can precise functional-group adsorption be achieved for 2D magnets
in experiment? Alloying is proposed to show potential for increasing the Curie temperature by theoretical predictions [245], so can
alloying be applied to 2D magnets in experiment, similar to those realized in traditional materials alloying? These exciting questions
and many other critical challenges await solid answers from the materials-synthesis community.
7.3. Flexible spintronics
Strain engineering is a popular method applied to 2D magnets for quantum phase transitions[159] and flexible electronics [355],
since the reduction in thickness of vdW materials to the atomic scale is often attributed to mechanical enhancement [104]. Until
recently, both experimental [356] and theoretical works [97,159] mainly focused on in-plane strain/stress modulation, which has
been introduced before in this review. However, the inhomogeneous deformation of 2D magnets lacks attention. For flexible spin
tronics, inhomogeneous deformations in the form of local curvature are ubiquitous at the nanoscale and often encompass exotic spin
states, such as topological or chiral spin states [357,358]. Chiral skyrmion and skyrmionium states can be achieved, engineered by the
gradient of curvature, which is contributed by the geometry-induced Dzyaloshinskii-Moriya interaction [359,360]. Simultaneously,
the size of skyrmions can be modulated by the curvature gradient as well [359,360]. The interplay of curvature and magnetism was
investigated in monolayer CrI3 and an accurate description of the flexomagnetic coupling parameters can be achieved [361]. The
controlled out-of-plane deformations and the measurement of the resulting bending for 2D materials can be fulfilled by aberration-
corrected, scanning transmission electron microscopy (STEM) [362]. Nevertheless, it is costly to study curved thicker membranes
by theoretical calculations, due to the costly nanotube geometry. Adapting so-called DFT methods, or treating curvature perturbatively
via flexural phonons, are alternative methods for considering curved effects in 2D magnets in calculations [361]. Therefore, focusing
on the curvature gradient of 2D magnets, apart from the in-plane stress–strain, holds great promise and opportunities for the potential
of flexible spintronics.
7.4. Multiferroics
The 2D multiferroics possesses different physical properties within one material, including ferromagnetism, ferroelectricity, fer
roelasticity and/or ferrovalley [363]. The origin and understanding of the cross-coupling phenomena of multiferroics has fascinated
physicists for decades, and the 2D multiferroics show great potential for spintronics [297,364]. However, the revealed 2D multiferroics
are rather limited, and research on the corresponding physical characteristics and possible applications is still in its infancy. The
challenges and opportunities in 2D multiferroics should be addressed.
1. It is still urgent to search for more 2D ferroics with high structural stability, high Curie temperature, and moderate switch barriers.
2D ferromagnets have been well-exploited and the research on ferroelectricity has gradually started, benefitting from machine
learning and high-throughput calculation methods [365,366]. In contrast, 2D ferroelastic and ferrovalley materials are rarely
explored by big-data filtering. Mining these materials by machine learning and high-throughput calculations can extremely
accelerate the exploration and achieving of more candidates for experimental preparation.
2. Switching a ferroelectric state or a multiferroic state with a voltage as small as 100 mV remains a great challenge. As the electric
field is proportional to the size of the ferroelectric, progress towards 100 mV switching voltage automatically requires either very
low switching fields or thick-enough length scales [367]. Therefore, understanding the ferroelectric switching behavior in the
ultrathin limit (less than20 nm) is critical [368].
3. Most 2D multiferroics have two polarization properties at the same time. For example, ferroelectric materials have both sponta
neous spin polarization and electrical polarization, and ferrovalley materials have spontaneous spin polarization and valley po
larization. However, few articles report 2D materials with three or more polarizations at the same time. Having more polarizations
simultaneously means that more couplings between different polarizations can be studied. For example, ferroelectricity and
antiferromagnetism can be coupled together by a ferrovalley in bilayer VS2 to realize an electronic control of magnetism [311].
Therefore, seeking multiferroics with more polarizations is of great significance for the study of novel physical phenomena of
multiferroic materials.
29
8. Conclusions and outlook
2D systems with possible long-range order in magnetization, polarization and other physical properties have been intensively
considered for their potential to break the Moore’s law limits in electronics and for application in spintronics. In addition to the charge
state, electron spins are exploited as a further degree of freedom, with implications in the efficiency of data storage, smart sensors, and
quantum computing. Recent breakthroughs achieved in 2D magnetic vdW crystals, in particular, the observation of room-temperature
2D magnetism, offer an ideal platform to understand the very basic “spin” of quantum matter.
Here we have reviewed magnetic properties in novel 2D vdW structures, including the background physics, particular structures,
external modulation and peculiar physical properties. A deep understanding of low-dimensional magnetism and the mechanism of
phase transitions is a necessary prerequisite for such an understanding. The spontaneous symmetry breaking of phase transitions,
renormalization theory, the Mermin-Wagner theorem and exchange interactions have been introduced. The discovered 2DFMs have
been systematically collated in other reviews before, from the perspective of symmetry and elemental composition. However, some
distinctive and ‘hot’ structures have been ignored which have rich physical properties; for instance, the proximity effect in hetero
structures and the colossal vertical electric field in Janus structures. Therefore, we emphatically review the recent progress in het
erostructures, Janus structures, nanoribbons and the recent star materials, MXenes and MBenes. To enhance the Tc and spin coupling,
modulation by an external field, strain, and crystalline engineering, including doping, grain boundaries and edges, have been discussed
in detail from the view of system symmetry breaking, which is the main focus in this review. The intriguing physical properties which
exist in 2DFMs are briefly introduced, for instance skyrmions and the QAHE, which are very appealing for data storage, quantum
computing and device transport.
Beyond these exciting achievements, the area of low-dimensional magnetism is still at a preliminary stage, which contains plenty of
opportunities and challenges. The first is the limitation of experimental methods to measure the magnetic properties, as small per
turbations will destroy the magnetism, such as thermal fluctuations, light exposure and inadvertent experimental preparation. Sec
ondly, theoretical development is immature as a guide to the enhancement of magnetic coupling. A great number of methods have
been proposed to increase the exchange interaction but still lack a unified theoretical explanation. Thirdly, the combinations of
theoretical predictions and experimental verification are insufficient. Although numerous candidates for 2DFMs have been screened
out with the assistance of density-functional calculations and machine-learning models, the results still need experimental verification.
It is believed that the development of room-temperature two-dimensional ferromagnetic materials will be greatly furthered by the
complementarity of experiments and theoretical calculations.
Declaration of Competing Interest
The authors declare that they have no known competing financial interests or personal relationships that could have appeared to
influence the work reported in this paper.
Data availability
Data will be made available on request.
Acknowledgements
This work was supported by the National Natural Science Foundation of China (51872017) and the high-performance computing
(HPC) resources at Beihang University.
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Progress in Materials Science 132 (2023) 101036

Contents lists available at ScienceDirect

Progress in Materials Science

Theory, properties and engineering of 2D magnetic materials

2DFMs 2D ferromagnetic materials

2.1. Spontaneously broken symmetries and phase transitions

2.2. Mermin-Wagner theorem

2.3. Magnetic anisotropy

where Zi is the atomic number, and ρ(ri ) is the charge density.

E = E0 + K2 sin2 θ + K4 sin4 θ (10)

2.4. Magnetic coupling model

2.4.1. Heisenberg model

2.4.2. Bond-dependent exchange (Kitaev model)

2.4.3. Antisymmetric exchange interaction

2.5. Layer-dependent effects

2.6. Fundamentals of symmetry breaking

2.6.1. Inversion symmetry breaking

2.6.2. Rotational symmetry breaking

2.6.3. Time-reversal symmetry breaking

2.6.4. Gauge symmetry breaking

3. Novel 2D ferromagnetic materials

3.1. Janus structures

Cr2C FM Half-metallic (2.85) [151] 672 Heisenberg model GGA + U [369]

4. Machine learning and high-throughput search for 2D magnets

4.1. High-throughput search

4.2. Machine learning

5. Modulation means for 2D magnets

5.1. Time-reversal and spontaneous gauge-symmetry breaking

5.1.1. Magnetic atom and carrier doping

5.1.2. Defect engineering

5.1.3. Surface decoration

5.2. Inversion symmetry breaking

5.2.1. Electric field

5.3. Rotational symmetry breaking

5.3.1. Strain engineering

5.4. Alloying and rare-earth atom doping

6. Intriguing physical phenomena for electronic devices

6.2. Quantum anomalous Hall effect

6.4. Magneto-optical effect

7. Opportunities and challenges

7.1. Fundamental theory

7.1.1. Mermin-Wagner theorem

7.1.2. Curie temperature

7.2. Synthesis and stability

achieve large-scale synthesis and industrialized mass production [345].

7.3. Flexible spintronics

8. Conclusions and outlook

Declaration of Competing Interest

Data will be made available on request.

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