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Recent Advances in Two-Dimensional Ferromag-

netism: Materials Synthesis, Physical Properties and
Device Applications
Pu Huang,a Peng Zhang,a Shaogang Xu,a Huide Wang,b Xiuwen Zhang∗a and Han
Zhang∗b

Nanoscale Accepted Manuscript

Published on 16 December 2019. Downloaded on 1/2/2020 [Link] PM.

Two-dimensional (2D) ferromagnetism is critical for both scientific investigation and technological
development owing to its low-dimensionality that brings in quantization of electronic states as well
as free axes for device modulation. However, the scarcity of high-temperature 2D ferromagnets
has been the obstacle of many researches, such as quantum anomalous Hall effect (QAHE)
and thin-film spintronics. Indeed, in the case of isotropic Heisenberg model with finite-range
exchange interactions as an example, low-dimensionality is shown to be contraindicated with
ferromagnetism. However, the advantages of low-dimensionality for micro-scale patterning could
enhance the Curie temperature (TC ) of 2D ferromagnets beyond the TC of bulk materials, opening
the way of designing high-temperature ferromagnets in 2D limit. In this paper, we review the
recent advances in the field of 2D ferromagnets, including their material systems, ferromagnetism
modulation, physical properties, and potential device applications.

1 Introduction
between spins located within individual planes of the crystal lat-
Ferromagnetism represents a form of magnetic order with the tice have been observed. 8,9 With the discovery of graphene, the
parallel alignment of intrinsic magnetic dipole moments or spin rapidly expanding family of 2D materials has been proven to have
of electrons in the crystal. 1 Ferromagnetic phases with sponta- excellent application prospects in many fields such as electron-
neous magnetization even in the absence of an external magnetic ics, 10–12 optoelectronics, 13–33 catalysis, 34–36 batteries, 37 super-
field, can be achieved from their high-temperature counter parts capacitors, 38,39 biomedicine, 40–46 sensing, 47–51 and ferromag-
possessing no macroscopic net magnetic moments. 2,3 The ferro- netism. 52 Meanwhile, with the development of epitaxial synthesis
magnetic state in three-dimensional (3D) materials, such as ele- and exfoliation techniques, the successful implementation of 2D
mental metals (e.g., Fe, Co, Ni 4 ) and their alloys, rare-earth met- materials (e.g., graphene, 26,53–56 TMDs, 57–60 topological insu-
als (e.g., Gd, Tb, Dy 5 ), and multicomponent compounds (e.g., lator, 61–63 black phosphorus, 11,64,65 Mxene, 66 antimonium, 67,68
LaMnO3 6 ) has been found for quite a long time, triggering ex- bismuth, 69 tellurium, 70–72 etc.) has become more and more sim-
tensive applications from the ancient compass to the modern ple and reliable, making its various related applications, espe-
data-storage devices. 7 In comparison with the investigation of cially the ferromagnetic applications, develop rapidly. These 2D
ferromagnetism in 3D materials, the research process on low- materials provide an exciting platform for studying the interplay
dimensional ferromagnets is relatively slow, although the begin- between various competing electronic and magnetic phenomena
ning of this kind of research can be traced back to 1970s 3 . Actu- at nanoscale involving the quantum confinement effect. Bene-
ally, two-dimensional (2D) ferromagnetism was initially probed fiting from the accelerating miniaturization of magnetic units in
in 3D crystalline magnetic materials, where distinct interactions spintronic devices, such as giant magneto-resistance, spin valve,
magnetic random-access memory (MRAM) and other spin logic
devices, 73 the studies of nano-magnetism are extremely vigorous
a
Shenzhen Key Laboratory of Flexible Memory Materials and Devices, College of Physics in recent years.
and Optoelectronic Engineering, Shenzhen University, Shenzhen 518060, China. E-
mail: xiuwenzhang@[Link] On the basis of Mermin-Wagner theorem, 77 short-range
b
Collaborative Innovation Centre for Optoelectronic Science & Technology, and Key isotropic interactions do not induce long-range order in low-
Laboratory of Optoelectronic Devices and Systems of Ministry of Educationand Guang- dimensional systems with continuous symmetry at finite tempera-
dong Province, International Collaborative Laboratory of 2D Materials for Optoelec-
tures, as demonstrated by the 2D isotropic Heisenberg model that
tronics Science and Technology of Ministry of Education, College of Physics and Op-
toelectronic Engineering, Shenzhen University, Shenzhen 518060, China. E-mail: does not have the ferromagnetic solution. In other words, realiz-
hzhang@[Link] ing the ferromagnetic coupling in 2D materials requires lowering

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DOI: 10.1039/C9NR08890C

Nanoscale Accepted Manuscript

Published on 16 December 2019. Downloaded on 1/2/2020 [Link] PM.

Fig. 1 (a) Layer-dependent magnetic ordering in atomically-thin CrI3 from monolayer (1L) to triple layer (3L). Adapted with permission. 74 Copyright
2017, Springer Nature. (b) Magnetic domain images of patterned Fe3 GeTe2 indicate that out-of-plane stripe contrast is weakened then evolves into
in-plane direction as the temperature increase from 220 K to 240 K. (c) Temperature dependence of the magnetic stripe contrast and the spatially
averaged contrast. [(b) and (c)] Reproduced with permission. 75 Copyright 2018, American Chemical Society. [(d) and (e)] The in-plane and out-of-
plane M-H loops for monolayer VSe2 on HOPG and temperature dependent magnetic properties of VSe2 films on MoS2 substrate. Adapted with
permission. 76 Copyright 2018, Springer Nature.

the symmetries, which is usually realized by the applied magnetic ery of intrinsic ferromagnetism in monolayer atomic crystals in
field or the inherent strong anisotropy of the crystal. Recently, Xu recent years. 74,77,78 The long-range magnetic ordering in 2D vdW
and Zhang et al. reported the ferromagnetic behavior in atomi- materials opens the door for exploring the low-dimensional fun-
cally thin layers of chromium germanium telluride (Cr2 Ge2 Te6 78 ) damental science and integrating the spintronic device seamlessly
and chromium triiodide (CrI3 74 ), using a polarmagneto-optical within 2D limit. Although great progress has been made via var-
Kerr effect microscopy technique. Moreover, room-temperature ious synthesis methods such as mechanical exfoliation from the
ferromagnetism was achieved in monolayer VSe2 . 76 These inspir- epitaxially grown bulk single crystal, 77 a great challenge still re-
ing results shed considerable light on seeking for new 2D ferro- mains hard to overcome for the achievement of tunable ferro-
magnetic materials, especially those with high Curie temperature magnetism, especially the control of the spin orientation, mag-
(TC ). More importantly, the in-depth physics about the sophis- netic domain phase, and the magnetic long-range order at ambi-
ticated palate of magnetoelectric interaction raises great interest ent temperature.
for the modern condensed matter physics.
In this review, we will focus on the recent progress on the
synthesis of 2D ferromagnets, magnetism-related phenomena, in- 2.1 Experimental synthesis and characterization
cluding but not limited to magnetic anisotropy, anomalous Hall Xu et al. 74 prepared the chromium iodide bulk crystals (CrI3 ) by
effect, magnetic phase transitions, gilbert damping etc., as well mixing chromium powder and anhydrous iodine beads, then ex-
as the 2D ferromagnetic devices, such as vdW heterojunctions foliated the CrI3 flakes from monolayer to few-layer structures
and spin valves. We attempt to summarize the underlying mag- with graphite encapsulation to prevent reaction with oxygen and
netic mechanism and issues that have not yet been uncovered moisture. The encapsulated CrI3 flakes present layer-dependent
for the associated 2D magnetic nanostructures. We believe that ferromagnetic phase transition from ferromagnetism in the mono-
the general insight into the 2D ferromagnetism not only provides layer, to antiferromagnetism in the bilayer, and back to ferromag-
guidelines for further engineering the magnetic properties, but netism in the trilayer and bulk [Fig. 1(a)]. Zhang et al. 75 fab-
also suggests promising candidates for future applications in spin- ricated bulk Fe3 GeTe2 crystal via chemical vapor transport, then
tronic devices. exfoliated thin Fe3 GeTe2 flakes (14-250 nm thick) on Si (111)
substrates. To facilitate the Fe3 GeTe2 exfoliation, they heated
2 Two-dimensional ferromagnetic material
the sample to 50 ◦ C and transfer the flakes into an ultrahigh
systems vacuum chamber (∼10−11 Torr). The subsequent measurements
Magnetic van der Waals (vdW) materials have emerged as show an enhancement of the perpendicular magnetic anisotropy
promising candidates for spintronic applications with the discov- in Fe3 GeTe2 microstructures, which undergoes transition from

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DOI: 10.1039/C9NR08890C

Nanoscale Accepted Manuscript

Published on 16 December 2019. Downloaded on 1/2/2020 [Link] PM.

Fig. 2 (a) Exfoliated layer ferromagnets, including CrI3 , Cr2 Ge2 Te6 and VSe2 . Adapted with permission. 74,76,79 Copyright 2018, Springer Nature. (b) In
situ observation of the unidirectional growth of h-BN domains and the shape evolution reproduced as a colour-coded superposition of outlines extracted
from images recorded during 760 s. Adapted with permission. 80 Copyright 2019, Springer Nature. (c) OM/AFM images of self-limited grown nonlayered
CdS flakes and the electron configuration of In/Cd-S motif on the flake surfaces. Reproduced with permission. 81 Copyright 2018, Wiley-VCH.

out-of-plane stripe domain phase to in-plane vortex phase at 230 its tunable magnetization characteristics below TC .
K and persists beyond room temperature [Fig. 1(b) and 1(c)].
Surprisingly, their result is opposite to conventional magnetic ma- Many issues remain in the materials preparation of 2D ferro-
terials for which finite-size microstructure leads to the reduction magnets, such as the controllable synthesis with high speed of
of TC . 86,87 However, the in-depth mechanism is still unclear and growth, large area realization and the stability under ambient at-
more detailed experimental and theoretical studies are required mosphere. Up to now, the commonly used method for prepar-
to explore the influence of finite size for vdW magnetic property. ing 2D ferromagnetic materials is mainly the mechanical exfolia-
McGuire et al. 88 mechanicaly exfoliated CrCl3 flake with scotch tion, 74,75,77,88 for which it is usually difficult to effectively control
tape onto 90 nm SiO2 substrates and obtained its 2D structures. the morphology, size and uniformity of layer thickness. Achieving
Furthermore, they observed a magnetic phase transition for CrCl3 the growth of large, high-quality single crystals of 2D components
flake with lowing temperature, which is attributed to the spin- (i.e., conductors, semiconductors, and insulators) is critical to the
lattice coupling within vdW interactions on the basis of DFT cal- industrial application of 2D devices in general. Therefore, explor-
culations. According to the previous experimental results, 89–92 ing a large-area controllable preparation method for 2D ferro-
bulk VSe2 exhibit paramagnetic characteristics, whereas ferro- magnetic materials is a challenge for current 2D ferromagnetic
magnetic transition can be induced when it is constrained into materials research. In fact, Liu et al. 80 have rencently realized
monolayer limit. 76 Batzill et al. 76 grew mono- and few-layer VSe2 the controllable epitaxial growth of single crystal monolayer h-
falkes on HOPG or MoS2 substrates by e-beam evaporation of V BN (∼100-square-centimetre) on a low-symmetry Cu (110) vic-
and simultaneous deposition of atomic Se from a hot wall Se- inal surface that is obtained by annealing an industrial copper
cracker source. After the HOPG or MoS2 substrates were trans- foil [Fig. 2(b)]. They revealed that the epitaxial growth can be
fered into the vacuum chamber and annealed in ultra-high vac- controlled by the coupling of Cu <211> step edges with h-BN
uum at 300 ◦ C for 5h, VSe2 began to grow with a slow rate of zigzag edges, which breaks the equivalence of antiparallel h-BN
∼0.06 ml min−1 . The following experiment measurements re- domains, enabling unidirectional domain alignment. This growth
vealed the strong ferromagnetic ordering with Curie temperature method is general for many other 2D material synthesis processes,
TC above room temperature (compared with its paramagnetic e.g., it is applied in realizing large area and high spead (60 µm/s)
bulk phase), 74 as shown in Fig. 1(d) and 1(e). Wang et al. 79 growth of graphene on Cu substrate. 93 These discoveries are ex-
mixed raw material powders of Cr, Ge, and Te with stoichiomet- pected to facilitate the widespread integration of two-dimensional
ric ratio [Link] for the growth of single-crystal Cr2 Ge2 Te6 by the devices and to achieve the epitaxial growth of a wide range of 2D
Te self-flux method. They applied the scotch tape approach to ob- materials. In addition to the common layered structure that can
tain few-layered Cr2 Ge2 Te6 from its bulk phase and demonstrate be easily exfoliated due to their relative low exfoliation energy,
one can also turn the attention to conventioal non-layered bulk

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orbital coupling (SOC) effect in the heavier iodine ions. Kan

et al. 82 proposed a double-orbital model and revealed that the
super-exchange-driven ferromagnetism is closely related to the
virtual exchange gap, i.e., the ferromagnetic coupling can be
increased significantly by lowering the gap with isovalent al-
loying [Fig. 3(a) to 3(c)]. Based on the model they pre-
dicted that the ferromagnetic coupling in monolayer CrWI6 and
CrWGe2 Te6 can be enhanced by 3∼5 times without introduc-
ing carriers. Petrovicet al. 83 observed a second-stage magnetic
transition in CrI3 below TC and described the low temper-
ature thermal demagnetization by the spin-wave model with
Moriya’s self-consistent renormalization. 101 They demonstrated
that the magnetic anisotropy in CrI3 comes predominantly from
the anisotropic symmetric super-exchange via Cr-I-Cr with large

Nanoscale Accepted Manuscript

SOC rather than the single ion anisotropy [Fig. 3(d) and 3(e)],
Published on 16 December 2019. Downloaded on 1/2/2020 [Link] PM.

which is in contrast with the arguement of Lado and Fernández-

Rossier. 99 Huang et al. predicted a series of 2D transition metal
magnetic compound, namely FeX2 , NiX2 , CoCl2 and CoBr2 mono-
layers (X = Cl, Br, I) that possess ferromagnetism, while VX2 ,
CrX2 , MnX2 and CoI2 are antiferromagnetic due to the compe-
tition between direct nearest neighbor d-d exchange and super-
exchange via halogen p state. 102 Victor Pardo et al. found a peri-
odic atomic distortion in VSe2 with 4 × 4 × 3 supercell by DFT
Fig. 3 [(a) to (c)] Schematic diagrams of the super-exchange interaction calculation, 103 which induces a strong reduction in the density of
and ferromagnetic coupling, including ferromagnetic/antiferromagnetic
states at the Fermi level and the non-magnetic phase transition.
alignments and exchange energy in CrI3 and CrGeTe3 monolayer. Re-
produced with permission. 82 Copyright 2018, American Chemical Soci- However, it should be noted that a huge discrepancy exists in the
ety. [(d) and (e)] Temperature-dependent reduced magnetization of CrI3 saturation magnetization between a monolayer VSe2 grown on
fitted using spin-wave model and (inset) single-particle model and the different substrate, e.g., VSe2 /MoS2 (15 µ B /V-atom) 76 and exfoli-
magnetic entropy change magnetization isothermals obtained by rotat-
ated multi-layer VSe2 (0.3×10−3 µ B /V-atom). 104 Moreover, pre-
ing from the ab plane to the c axis in various fields. 83 Copyright 2018,
American Physical Society. vious DFT calculations of bulk and monolayer VSe2 show that the
ferromagnetic phase is the most stable structure, 105,106 whereas
the values of magnetic moment is in significant disagreement with
materials. Although it is difficult to directly obtain their atomic experimental results.
layers due to the challenge of breaking the instrinsic isotropic Above all, the theoretical exploration about 2D ferromagnetism
chemical bonds and the unsaturated dangling bonds on the sur- is still on the way with many issues and puzzles required to be
face, which usually increase the system total energy significantly clarified. We believe further detailed investigations are needed
and make the structure unstable. Nevertheless, it is still possible to probe the inter/intra-layer interaction and the origin of ferro-
to obtain the ultra-thin monolayer 2D flake via self-limited epi- magnetism within 2D limit. Especialliy, a relatively general model
taxial growth, 81,94 which apparently enriches the research scope is needed to describe the complicated ferromagnetic interaction,
of 2D ferromagnets beyond vdW layered materials [Fig. 2(c)]. which is not only the recognition of magnetic mechanism but also
The synthesis of 2D ferromagnetic materials could benefit from crucial to predict or design new 2D ferromagnets. In addition,
the analysis of structural symmetry, atomic bonding characteris- influence of substrate or other external perturbations to the mag-
tics for individual crystal surface and vdW interface, uncovering netic stability need be considered, as strain are capable to destroy
the atomic arrangement and magnetic domain evolution, which the magnetism. 106
is cricital for realizing the controllable synthesis of 2D ferromag-
nets. Furthermore, the cooperation of theory and experiment 3 Modulation of ferromagnetism in 2D ma-
would greatly promote the research progress of 2D ferromagnetic terials
materials, especially the adoption of high-throughput (HT) calcu-
lation, HT experiment and machine learning 95–98 methods could 3.1 Magnetic doping
accelerate the design of new high-temperature 2D ferromagnets. Defect doping, which is the intentional introduction of impurity
element into a material, plays a significant role in functionalizing
2.2 Theoretical investigation and prediction 2D systems by changing the intrinsic properties of pristine atomic
On the basis of DFT calculations, Lado and Fernández-Rossier 99 layers. 107,108 Magnetic dopents (e.g., Fe, Co, Ni, Mn etc.) interca-
suggested that the large magnetic anisotropy in CrI3 origi- lated into 2D transition-metal dichalcogenides (TMDs) have been
nates from an anisotropic exchange interaction through a super- promising as diluted magnetic semiconductors and some of them
exchange mechanism, 100 which stems from the strong spin- have been predicted to exhibit ferromagnetic behavior at room

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Nanoscale Accepted Manuscript

Published on 16 December 2019. Downloaded on 1/2/2020 [Link] PM.

Fig. 4 [(a) and (b)] AFM and Raman spectra of the Fe0.021 Sn0.979 S2 and SnS2 monolayer. [(c) and (d)] Magnetic hysteresis loops measurement at 2 K
using vibrating sample magnetometer and schematic of the Fe 3d electron arrangement with spin in Fe-SnS2 . [(a) to [d]] Adapted with permission. 84
Copyright 2018, Springer Nature. (e) Schematics of the MBE syntheszed MSi2 silicene at the Si (111) substrate and the structural characterization,
including RHEED and X-ray diffraction scan image of 4-5 layer GdSi2 and HAADF-STEM image of monolayer GdSi2 . [(f) and (g)] Temperature
dependence of the AFM/FM magnetic moment in bulk GdSi2 and 4-5 layer GdSi2 . [(e) to (g)] Adapted with permission. 85 Copyright 2018, Springer
Nature. (h) Schematic illustration of the synthesis process for F-antimonene. [(i) and (j)] The wide range (2-800 K) M-T measurements to determine TC
of F-antimonene and pure antimonene. [(h) to (j)] Reproduced with permission. 52 Copyright 2019, Wiley-VCH.

temperature. For instance, transition metal (e.g., Nb, Co, Mn) tals using adhesive tape and deposited on either SiO2 /doped
doped MoS2 nanosheets, 60,109,110 Fe doped SnS2 84 have been Si substrate or polydimethylsiloxane (PDMS) sheets. Magneto-
synthesized via the chemical vapor deposition method and pro- transport in the exfoliated tens of nanometers thick flakes re-
vide the possibility of electronic control of magnetism. However, vealed ferromagnetic ordering below its Curie temperature TC
complete understanding the in-depth micro-mechanism about the (∼110 K) as well as strong in-plane magnetic anisotropy. Stor-
defect induced magnetic properties in 2D systems still requires chak et al. 85 functionalized layered silicene with rare-earth atoms
further researches. (Gd and Eu) ranging from the bulk down to one monolayer and
found the evolution from the antiferromagnetism of the bulk to
Wu et al. 111 investigated the magnetism of Fe-doped SnS2 in intrinsic 2D in-plane ferromagnetism of ultrathin layers [Fig. 4(e)
details and demonstrated that the ferrimagnetism originates from to 4(g)]. Zeng et al. 113 predicted a series of stable 2D transi-
the exchange interaction between intralayer Fe atoms, whereas tion metal dihydride (MH2 , M=Sc, Ti, V, Cr, Fe, Co, Ni) with
interlayer Fe interaction lead to paramagnetic state. Wei et al. 84 ferromagnetic or antiferromagnetic characteristics. Among them,
mixed Sn, S, and FeCl3 powders in different stoichiometrics and monolayer CoH2 is a ferromagnetic metal with room-temperature
obtained Fe-doped SnS2 via the direct vapor transport technique TC (339 K), while ScH2 can possess half-metallicity through hole
[Fig. 4(a) to 4(d)]. Finally, they realized Fe doped SnS2 in doping and keep a relatively high TC (160 K). Moreover, they
experiment and proved that long-range ferromagnetic ordering proposed a synthetic approach to realize CoH2 and ScH2 mono-
(TC 31K) in the Fe-doped SnS2 monolayer is energetically stable layers in experiments. González-Herrero et al. 114 demonstrated
according to DFT calculations. Yamasaki et al. 112 fabricated bulk that a magnetic moment can be induced in hydrogen adsorbed
crystals of Cr1/3 TaS2 and Fe1/4 TaS2 by chemical vapour trans- graphene with a ∼20 meV spin splitting state at the Fermi energy.
port, then exfoliated thin flakes of the materials from bulk crys-

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Based on scanning tunneling microscopy detections and DFT cal-

culations, they found that such a spin-polarized state is essentially
localized on the carbon sublattice opposite to the chemisorbed hy-
drogen site, forming extended spin textures and direct coupling
between the magnetic moments at unusually long distances.

3.2 Non-magnetic doping induced magnetic ordering

The above mentioned 2D ferromagnetic materials involve the el-
ements with valence d-electrons or f-electrons, such as Cr, Fe,
Co, and Eu, with magnetic ordering originated from the partially
filled d-bands or f-bands. On the other hand, materials based
on elements with only sp-valence electrons could also have spin
splitting and magnetic ordering in certain circumstances−these
materials can have high magnitudes of spin-wave stiffness, 115

Nanoscale Accepted Manuscript

Published on 16 December 2019. Downloaded on 1/2/2020 [Link] PM.

leading to potentially higher Curie temperature. The ferromag-

netism as well as anti-ferromagnetismin in graphene-related ma-
terials have been studied extensively, 116 induced by defects, grain
boundaries, nanostructure boundaries, etc. Zhao et al. 117 real-
ized ferromagnetism in BN nanosheet with random substitution
of B and/or N atoms by C atoms, suggesting a Curie tempera-
ture higher than 400 K. Tang et al. 52 studied the magnetic prop-
erties of the air-stable few-layer antimonene under fluorination,
revealing a robust ferromagnetism with Curie temperature of 717
K, induced by the low-density sp-electron spin-polarized impu-
rity sub-bands [Fig. 4(h) to 4(j)]. Louie et al. 118 found that
tunable ferromagnetism and half-metallicity can be induced in
monolayer GaSe by carrier (hole) doping. The averaged electron
spin magnetic moment per carrier reaches a plateau near 1.0 µ B , Fig. 5 (a) Crystal structures of transition-metal oxyhalides and the Curie
leading to a half-metallic state of GaSe, then descends abruptly. temperature comparison between CrOCl under 5% biaxial tensile strain
They demonstrated that this itinerant magnetism originates from and recently discovered 2D ferromagnetic compounds. Reproduced with
a Stoner mechanism with an exchange-field splitting of the elec- permission. 119 Copyright 2018, American Chemical Society. [(b) and (c)]
Total exchange energy, magnetic anisotropicenergy and magnetic mo-
tronic states near the VBM, where the density of states are very ment per site as a function of temperature for monolayer CrI3 , CrWI6 and
high and exhibits a sharp van Hove singularity. 118 These stud- CrWGe2 Te6 (under 4% tensile strain case) from Monte-Carlo simulations.
ies demonstrate that the non-magnetic dopants in non-magnetic Reproduced with permission. 82 Copyright 2018, American Chemical So-
materials could favor spontaneous spin polarization and local mo- ciety.
ment formation, as well as long-range magnetic ordering.

sustain external strains up to 11% and 6%, respectively. 120,121,125

3.3 Strain modulation The softness of single layer 2D structure implies that strain engi-
It has been demonstrated that strain engineering can effectively neering of their electronic and magnetic properties can be real-
tune the electronic characteristics for low-dimensional materials ized in these systems. Indeed, Miao et al. 119 proposed a promis-
(e.g., using substrate lattice mismatch 59,120,121 ). For 2D mate- ing alternative way to create 2D intrinsic ferromagnetism from
rial family, strain engineering has been used as a powerful tech- bulk vdW antiferromagnets, as realized in the CrOX monolayers
nique to tune their physical quantities and generate novel prop- which can be easily exfoliated from their bulk counterparts. The
erties, such as band gap, carrier mobility and excitonic absorp- robust long-range ferromagnetic ordering lies in the out-of-plane
tion. 59,122,123 Moreover, structural deformation induced by ex- direction of 2D CrOX, indicating the easy magnetization axis with
ternal strain also has an influence on the magnetic stability. It large spin polarization and magneto-crystalline anisotropy energy
is known that magnetic anisotropy energy defines the stability of [Fig. 5(a)]. Moreover, under appropriate strains, the TC of CrOX
magnetization in a specific direction with respect to the crystal monolayers can be further enhanced up to 204 K. Kan et al. 82
lattice and is an important parameter for spintronic applications. have predicted the room-temperature ferromagnetic phase transi-
Hence, magnetic characteristics (e.g., anisotropy and TC ) modu- tion for monolayer CrWI6 and CrWGe2 Te6 under a small in-plane
lated by strain has become a subject of field-regulated ferromag- ∼4% tensile strain [Fig. 5(b) and 5(c)]. Lam et al. 126 demon-
netism recently. strated that monolayer chromium trihalides CrX3 (X = Cl, Br, I)
In general, 2D atomic structures possess the unique mechani- are soft with 2D Young’s modulus of 34, 29 and 24 N/m through
cal advantage and can usually sustain larger strains than their 3D DFT calculations. In particular, all three compounds exhibit ferro-
bulk counterpart. 124 For instance, single-layer MoS2 and FeSe can magnetic ordering under zero strain, whereas their antiferromag-

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netic phase transition occurs upon a compressive strain, which is precise thresholds for such electric switching of magnetic order
demonstrated by Webster et al. 127 They further revealed a strain depend on the specific twist angle (≤2◦ ). 55 However, other cru-
dependence magnetic anisotropy in the CrX3 , i.e., the anisotropy cial details such as longer-range interactions, spontaneous defor-
is enhanced with compressive strains for CrI3 , which is opposite mations and interlayer screening etc., have not been considered
for CrBr3 and CrCl3 . 126 and needed to be further studied.

4 Physical properties of 2D ferromagnetic

3.4 Electric field modulation
materials
Manipulating a quantum state via electrostatic gating has been
of great importance for many model systems in nanoelectron- 4.1 Magnetic anisotropy: the condition needed for 2D ferro-
ics. 128,129 However, the effective tuning of the electron spins magnetism
or the magnetism of a system by external electric field has In the realm of 2D ferromagnetism, the magnetic anisotropy is the
been challenging. Wang et al. 79 prepared exfoliated few-layered critical factor because it prevents the random spin reorientation
Cr2 Ge2 Te6 from its single-crystal using the scotch tape method, induced by thermal fluctuation. 77 The anisotropy mainly comes

Nanoscale Accepted Manuscript

then deposited it onto silicon oxide with h-BN encapsulation. from the lattice structure of the material itself, so that the Heisen-
Published on 16 December 2019. Downloaded on 1/2/2020 [Link] PM.

They found that the layered Cr2 Ge2 Te6 devices possess tunable berg model with SOC possesses single-ion anisotropy, which de-
magnetism via gating, as characterized by micro-area Kerr mea- stroys the isotropy of the Hamiltonian and induce 2D ferromag-
surements below TC [Fig. 6(a) and 6(b)]. They attributed the netism. Extensive theoretical and experimental efforts 74,82,119
observed bipolar magnetism tunability to the rebalance of spin- have been made to enhance the magnetic anisotropy of the mag-
polarized band structure with shifting Fermi level. Xu et al. 130 netic nanostructures to promote the stability of the magnetiza-
found the electrostatic gate control of magnetism in CrI3 bilay- tion, for the potential applications at high temperature. Gen-
ers using magneto-optical Kerr effect (MOKE) microscopy [Fig. erally speaking, magnetic anisotropy depends on two factors:
6(c) and 6(d)], revealing the switching between antiferromag- the spin-orbit coupling which contributes magneto-crystalline
netic and ferromagnetic states realized by external voltage. They anisotropy and the magneto-static dipole-dipole interaction. The
further demonstrated the spin-layer locking induced by a time- magneto-crystalline anisotropy usually occur at a surface or in-
reversal pair of layered antiferromagnetic states, which leads to terface 134,135 owing to the lack of neighbors and the lowered
a linear dependence of their MOKE signals on gate voltage with symmetry, which is evaluated by the magnetic anisotropy energy
opposite slopes. Mak et al. 131 fabricated dual-gate field-effect de- (EMAE ). The reliable determination of EMAE for a given material
vices of atomically thin CrI3 with h-BN as the gate dielectrics and requires highly accurate electronic structures and proper treat-
few-layer graphene as the gate and contact electrodes, realizing ment of the weak SOC Hamiltonian. Thus, non-collinear non-
the control of magnetism in bilayer antiferromagnetic CrI3 via us- selfconsistent calculations are necessary to evaluate the total en-
ing a small gate voltage. They proposed that the external elec- ergies after the self-consistent ground states were achieved. Ac-
tric field creates an interlayer potential difference, which leads to cording to the magnetic anisotropy theorem, the EMAE can be
a linear magnetoelectric effect and interlayer spin-flip transition determined by the formula EMAE =E(→)−E(↑), where the arrow
[Fig. 6(e) to 6(g)]. Furthermore, they demonstrated that elec- indicates the direction of magnetization. Usually for 2D system,
trostatic doping can effectively modify the magnetic properties of the formula can be rewritten as EMAE =E(0◦ )− E(90◦ ), where the
both monolayer and bilayer CrI3 by using CrI3 /graphene vertical E(θ ) is the computed total energies from the Kohn-Sham equa-
heterostructures. 132 tions as a function of the angle θ between the magnetic moment
and the atomic plane. EMAE <0 (>0) describes an in/out-of plane
As to monolayer CrI3 , hole/electron doping significantly
easy-axis situations (parallel or perpendicular to the 2D system),
strengthen/weaken the magnetic order by modulating the sat-
respectively.
uration magnetization, coercive force, and TC . 132 Remarkably,
the moderate electron doping (above ∼2.5×1013 cm−2 ) can in-
duce a ferromagnetic transition for bilayer CrI3 [Fig. 7(a) to 4.2 Magnetic proximity effect
7(d)]. They emphasize the strongly doping-dependent interlayer Benefit from the fabrication of 2D atomic heterostructures, prox-
exchange coupling, which can be used to realize the switching of imity effect becomes prominent and can be used to tune the
magnetization in bilayer CrI3 . Zhang et al. 133 demonstrated that characteristics of pristine layer. 136 Proximity effect can drive a
the ferromagnetic transition temperature of layered Fe3 GeTe2 is given material forming superconducting, 137–139 magnetic, 140,141
suppressed compared with its bulk (205 K) [Fig. 7(e) to 7(g)], or topologically states, 142,143 through the adjacent regions. In
the ionic gate can significantly raise TC to room temperature. 133 bulk materials, the sample size could dwarf the characteristic
San-Jose et al. 55 found that two types of magnetic order in bi- lengths of proximity effects which usually can be ignored. How-
layer graphene, i.e., lattice antiferromagnetism and spiral ferro- ever, in monolayer vdW limit such as graphene or TMDs, the
magnetism, are both concentrated at AA-stacked regions and can situation is different; even short-range magnetic proximity ef-
be switched by a vertically electrical field. Ferromagnetic polar- fects exceed their thickness. Taking advantage of the magnetic
ized AA regions evolved into spiral magnetic ordering, keeping a proximity effect, Leutenantsmeyer et al. 144 presented the direct
relative 120◦ misalignment between neighboring regions due to measurement of room temperature ferromagnetism in graphene
a frustrated antiferromagnetic exchange. They suggested that the by spin transport. Wang et al. 140 placed graphene on an atom-

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Nanoscale Accepted Manuscript

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Fig. 6 [(a) and (b)] Electrical transport and magnetic properties of Cr2 Ge2 Te6 FETs and the renormalized Kerr angle measured at 20 K with fixed ionic
gate voltages of 0, -2 and -4 V. Adapted with permission. 79 Copyright 2018, Springer Nature. [(c) and (d)] Intensity of the polar MOKE signal of a
non-encapsulated bilayer CrI3 device as a function of gate voltage and magnetic field and the gate-induced variation of the metamagnetic transition at
-50 V, 0 V and 50 V. Adapted with permission. 130 Copyright 2018, Springer Nature. (e) AFM bilayer CrI3 consists of two FM monolayers with an AFM
interlayer coupling and zero net magnetization. [(f) and (g)] Electrical switching of the magnetic order in bilayer CrI3 and the MCD signal as a function
of magnetic field under representative electric fields. [(e) to (g)] Adapted with permission. 131 Copyright 2018, Springer Nature.

ically flat yttrium iron garnet (YIG) ferromagnetic thin film and and found that the magnetic proximity effect results in a strong
demonstrated that the anomalous Hall conductance can be kept Zeeman splitting in graphene with the exchange field up to hun-
up to ∼300 K. Katmis et al. 145 demonstrated the topologically dreds of tesla, which leads to the transformation from a quan-
enhanced interface magnetism by coupling a ferromagnetic insu- tum Hall state into a ferromagnetic state or a canted antiferro-
lator (EuS) to a topological insulator (Bi2 Se3 ) in a bilayer sys- magnetic state. Inyang et al. 153 determined the scaling between
tem by using the spin-polarized neutron reflectivity experiments, the proximity-induced magnetization in Pt and the temperature
which persists up to room temperature. Scharf et al. 146 provided dependent interface magnetization for the adjacent ferromag-
the description of Coulomb interaction in magnetic proximity ef- net, which is induced by the effective magnetic susceptibilities of
fects and elucidated how they transform the neutral excitons X0 heavy metal and is in contrast with the generally expected linear
in TMDs on magnetic substrates (from dark to bright state). Yang scaling for ferromagnet interface magnetization. Karpiak et al. 154
et al. 147 reported that a strong spin polarization of π orbitals in evidenced the existence of an out-of-plane proximity-induced fer-
graphene can be induced through the interaction with EuO mag- romagnetic exchange interaction between graphene and mag-
netic insulator due to the magnetic proximity effect, which results netic insulator Cr2 Ge2 Te6 , as the lifetime for perpendicular spins
in 24% spin polarization of the orbitals and a large exchange- are much longer than the in-plane counterpart, which indicates
splitting band gap (36 meV). They further revealed the possi- the proximity-induced anisotropic spin texture in graphene. A
ble engineering of graphene spin-gating by proximity of a few general theory has recently been established to extract the ex-
magnetic insulators, including EuO, EuS, YIG and cobalt ferrite change coupling fields induced by proximity through the Hanle
(CFO). 148 Usually the adjacent magnetic insulator could induce spin precession analysis. 155 Most recently, Tong et al. 156 found
magnetic exchange field and enable efficient control of local spin that the magnetic proximity effect in vdW moiré superlattice de-
generation and modulation without compromising the material pends sensitively on the interlayer atomic registry due to the spin-
structures. Using graphene/EuS heterostructure, Wei et al. 149 dependent interlayer orbital coupling. The spatial variation of the
demonstrated that the coupling between graphene and magnetic atomic distribution leads to a lateral modulation of a magnetic
insulator produces a substantial magnetic exchange field (>14 proximity field and generates a miniband spin splitting, which
T), which leads to significant enhancement of the spin signal orig- strongly depends on the moiré periodicity and can be tuned me-
inating from the Zeeman spin Hall effect. Lazić et al. 150 showed chanically by a relative twisting and/or strain between the vdW
the tunable magnetic proximity effect in 2D heterostructures due layers. They further showed the effective modulation of mini-
to the vdW bonding interaction, which both modulates the mag- band spin splitting via a perpendicular electric field because of
nitude of spin polarization and enables its sign change in ph- the modulation on the interlayer distance.
ysisorbed graphene, e.g., Co/bilayer graphene, Co/BN/graphene,
and Co/BN/benzene. Eremeev et al. 151 found that the charge 4.3 Quantum anomalous Hall effect
redistribution and orbital mixing between the topological insu-
The theoretical discovery of topological phases 157,158 substan-
lator and magnetic insulator at the interface cause drastic mod-
tially advanced the condensed matter physics, leading to deeper
ifications of the electronic structure due to magnetic proximity
understanding of materials for technological applications. The
effect. Wu et al. 152 fabricated graphene-BiFeO3 heterostructures
intriguing quantum anomalous Hall state was predicted by Hal-

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DOI: 10.1039/C9NR08890C

Nanoscale Accepted Manuscript

Published on 16 December 2019. Downloaded on 1/2/2020 [Link] PM.

Fig. 7 [(a) to (d)] Schematic side view of a dual-gate bilayer CrI3 field-effect device (left upper panel), doping density-magnetic field phase diagram
(right upper panel), interlayer exchange constant J⊥ and spin-flip transition field Hsf as a function of gate voltage and gate induced doping density (lower
panels). The gate-voltage controlled MCD is obtained from monolayer CrI3 at 4 K. Adapted with permission. 132 Copyright 2018, Springer Nature. (e)
Atomic structure and optical image of few-layer Fe3 GeTe2 flakes exfoliated on top of Al2 O3 thin film. (f) Phase diagram and coercive field as the gate
voltage. (g) Hall resistance Rxy of few-layer Fe3 GeTe2 as a function of magnetic field with different gate voltages obtained at T = 10 K and 240 K. [(e)
to (g)] Adapted with permission. 133 Copyright 2018, Springer Nature.

dane in 1988, 159 and was realized in experiment in 2013 by in- with a Curie temperature of 27 K. Combined experiments with
troducing magnetic dopants in the 2D form of a 3D topological theoretical calculations, Tian et al. 166 revealed the strong topo-
insulators with a small energy gap opened between the topologi- logical character of MnBi6 Te10 possessing Dirac surface states,
cal surface states at 30 mK. 160 Significant efforts have been made which can evolve into the antiferromagnetic topological insula-
to raise the critical temperature of QAHE state. 161 Qiao et al. 162 tor phase at T<10.8 K. Moreover, the ferromagnetic axion in-
found from theoretical calculations that graphene on the (111) sulator phase emerges at small field (0.1 T) and leads to a sat-
surface of room-temperature multiferroic BiFeO3 can host the urated anomalous Hall resistivity up to 10 K, which can also
QAHE state due to the magnetic proximity effect plus the topo- be preserved even when external field decreases to zero at 2 K.
logical band structure of graphene. Similarly, Zhang et al. 163 Hao et al. 167 revealed a gapless surface Dirac cone in single crys-
predicted robust QAHE in the vdW heterostructure formed by tal MnBi2 Te4 using high-resolution angle-resolved photoemission
graphene and 2D Cr2 Ge2 Te6 with a relatively high Curie tempera- spectroscopy (ARPES) characterization and first principles calcu-
ture of 61 K. The experimental attempts on this type of graphene- lation, which is quasi-2D and stable under massive surface ab-
based heterostructures demonstrate anomalous Hall conductance sorbents. Through magneto-transport, bulk magnetization and
approaching the QAHE conductance. 164 Chen et al. 165 predicted neutron scattering measurement, Wang et al. 168 investigated the
the QAHE state in intrinsically ferromagnetic CoBr2 monolayer magnetic and transport properties for trigonal Cr5 Te8 single crys-

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tals and demonstrated the appearance of topological Hall effect of magnons has been proven in an antiferromagnetic TlCuCl3
with current along the c axis and field in ab plane, which stems compound at low temperatures by Nikuni et al. 187 Further, room
from the noncoplanar spin configurations with scalar spin chiral- temperature magnons in YIG films were reported by Demokri-
ity during the spin flop process. Chen et al. 169 reported the ferro- tov et al. 188 Uchida et al. observed the generation of spin cur-
magnetic vdW compound MnSb1.8 Bi0.2 Te4 (TC =26 K) with excess rents in Pt/BiY2 Fe5 O12 interface with Au nanoparticles embed-
anomalous Hall signal which is beyond the conventional AHE. Re- ded in the BiY2 Fe5 O12 layer. 189 They suggested the spin-current
cently, numerous topological materials have been predicted from generation originates from non-equilibrium magnons excited by
high-throughput calculations 170–172 −the combination of strong surface plasmon induced evanescent electromagnetic fields in
SOC with spatial anisotropic in their 2D structures could rend BiY2 Fe5 O12 . Balatsky et al. 190 found that Coulomb interac-
them candidate base materials for QAHE phases, opening the tions between fermions in honeycomb layered chromium tri-
arena for the design of high-temperature QAHE materials. halides induce strong temperature and momentum-dependent
renormalization of the magnon bands near a Dirac cone, thus
4.4 Giant magnetoresistance clarify the long debated puzzle of spin-wave anomalies in
CrBr3 . 191,192 Ghazaryan et al. 193 studied the tunneling effect
Giant magnetoresistance is a quantum mechanical magne-

Nanoscale Accepted Manuscript

in graphene/CrBr3 /graphene vdW heterostructures and demon-
Published on 16 December 2019. Downloaded on 1/2/2020 [Link] PM.

toresistance phenonmena discovered by Albert Fert and Peter

strated that the inelastic tunneling through thin ferromagnetic
Grünberg, 173,174 which presents a significant change in the elec-
CrBr3 barriers are mainly associated with magnon emission at low
trical resistance when the magnetization of adjacent ferromag-
temperature, i.e., the spin state (up or down) of a tunneling elec-
netic layers transfer between parallel and antiparallel alignments.
tron will be flipped between the initial and final states during the
The giant magnetoresistance effect is based on the dependence of
magnon process. Very recently, Xing et al. 194 reported the exper-
electron scattering on the spin orientation and offers a new knob
imental observation of long-distance magnon propagation over
to control the overall resistance via manipulating magnetization
several micrometers in quasi-two-dimensional vdW antiferromag-
direction, which lays the foundation of modern data storage tech-
net MnPS3 , which is comparable to the bulk ferromagnetic insu-
nology, such as hard disk drives, 175,176 biosensors, 177 microelec-
lator YIG. They demonstrated that the magnon diffusion length
tromechanical systems (MEMS) and other devices. 178 This effect
is sensitive to temperature and layer thickness, which could be
has also been extended to 2D ferromagnets, and exhibit more
attributed to the surface impurity-induced magnon scattering.
novel features. Xu et al. 179 fabricated multiple spin filtermag-
netic tunnel junctions composed of graphene/CrI3 /graphene vdW
heterostructures, revealing a drastical enhancement (19000%) of 4.6 Anisotropic Gilbert damping
tunneling magnetoresistance for the four-layer device at low tem- Gilbert damping is a fundamental parameter in magnets and de-
peratures, which is significantly larger than conventional barrier- scribes the relaxation of magnetization to the equilibrium con-
based ferromagnetic tunnel junctions (e.g., MgO 180,181 ). They stant value, which determines the performance of many spin-
attributed these effects to the intrinsic interlayer antiferromag- tronic devices. 195–197 Based on the SOC band structure in regard
netic ordering of the atomically thin CrI3 . Wang et al. 182 found of the orientation of magnetization direction, theoretical works
that tunneling conduction in the direction perpendicular to the suggested that damping should be anisotropic in single-crystalline
exfoliated CrI3 crystalline planes exhibits a ten times magnetore- ferromagnetic metals (e.g., Fe, Co, Ni). 4 However, electron scat-
sistance enhancement, which originates from multiple transitions tering will dramatically reduce the anisotropic characteristics
between different magnetic states as characterized by the evolu- with the smearing of energy bands, leading to the challenge for
tion of magnetoresistance with magnetic field and temperature. direct observation of anisotropic damping in 3D bulk. Only a few
On the basis of tight-binding model and DFT calculation, Zhong experiments attempted to prove this phenomena, whereas con-
et al. 183 demonstrated a giant magneto bandstructure effect dom- vincing evidence is still lacking. Until most recently, Back et al. re-
inated significantly by the magnetization direction. Through the ported the emergence of anisotropic magnetic damping in 2D fer-
analysis while rotating the magnetic moment of CrI3 from out-of- romagnetic metal/semiconductor interface of Fe/GaAs(001) het-
plane to in-plane, they observed a direct-to-indirect band struc- erojunction. 198 They demonstrated that the fourfold symmetry
ture transition, which indicates the magnetic field controlled pho- exists in the Fe/GaAs(001) heterojunction, thus no in-plane dis-
toluminescence. tortions occur, which is different from Fe/InAs(001) where there
is structural anisotropy originating from crystal growth. 199,200
4.5 Magnon Through DFT calculation, they further attributed the anisotropic
Gilbert damping to interfacial symmetry-breaking of Fe atoms in
Magnon represents a collective behavior of magnetic moments
light of the rapidly reduction of anisotropy with increasing Fe film
in a specific system, which can generally be treated as one com-
thickness.
plete precession distributed over a chain of spins (a quantized
spin wave) and obeys the Bose-Einstein statistics. 184 The con-
trol of magnon-mediated spin current is useful for information 4.7 Circular optical polarization
logic device and computing applications. 185 Magnon was firstly Ferromagnets give rise to time reversal symmetry breaking due
detected in experiment by Brockhouse et al., 186 using the in- to the inherent spontaneous magnetization. The observation of
elastic neutron scattering method. Bose-Einstein condensation net circular polarized emission provides a convinent probe for

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Nanoscale Accepted Manuscript

Published on 16 December 2019. Downloaded on 1/2/2020 [Link] PM.

Fig. 8 (a) Schematic of magnetic states in bilayer CrI3 , the 2D spin-filter magnetic tunnel junction and its tunneling current at selected magnetic
fields. 179 Copyright 2018, American Association for the Advancement of Science. (b) Optical micrograph of a tetralayer CrI3 tunnel junction and
conductance through a bilayer and tetralayer CrI3 tunnel barrier as a function of an out-of-plane applied magnetic field. 201 Copyright 2018, American
Association for the Advancement of Science. (c) Bilayer WTe3 /Permalloy sample geometry and schematic of the spin-orbit torque measurement system.
Adapted with permission. 202 Copyright 2018, Springer Nature. (d) Schematics of a spin field-effect transistor based on 2D antiferromagnetic half metals
and its predicted spin-polarized current. 203 Copyright 2018, National Academy of Sciences. (e) vdW spin valve structure, where the 2D conductor is
sandwiched between two ferromagnets. The magnetization of the bottom ferromagnetic layer is pinned, whereas the top layer can switch, resulting in
parallel and antiparallel states with distinct in-plane conductance. 204 Copyright 2018, American Physical Society.

the appearance of spontaneous magnetic ordering. In fact, inves- spin-dependent charge hopping across the heterostructure inter-
tigation about the interaction between ferromagnet and circular face.
polarized response was initialized in 3D heterojunction and has
been extensivly studied for many years. 205,206 Jonker et al. 207 4.8 Current-induced spin-orbit torques
injected the spin-polarized electrons into Si (001) from an iron
Current-induced spin-orbit torques (SOTs) in inversion-
film through an Al2 O3 tunnel barrier. They found that the cir-
asymmetric system has emerged as a scientific and technological
cular polarization of the electroluminescence resulting from ra-
interests in recent years. 210 The manipulation of magnetic
diative recombination traces the Fe magnetization, thus confirm-
characteristics by SOTs evidences the microscopic interactions
ing that these spin-polarized electrons originate from the Fe con-
between charge and spin in a variety of materials and enables
tact. Also the circular polarized electroluminescence was deter-
the designing of spintronics with potentially applications in data
mined in III-V heterostructures with p-type ferromagnetic semi-
storage, low-power memory and logic devices. Garello et al. 211
conductor as the spin polarizer. 208 With the rapid development
provided a general scheme to measure the amplitude and direc-
of low dimensional materials, the research scope is extended to
tion of SOTs and demonstrated that heavy-metal/ferromagnetic
magneto-optical interaction within the 2D limit. Most recently, Xu
layers present different SOTs with odd and even behaviour con-
et al. 209 reported the intimated connection between magnetiza-
sidering their magnetization reversal. They found such torques
tion direction and circularly polarized photoluminescence in CrI3 .
possess strongly anisotropic field-like and spin transfer-like
The circular polarization exists in monolayer ferromagnetic form,
components, which is determined by the type of heavy-metal
whereas vanishes in bilayer antiferromagnetic structure. They
layer and annealing treatment. Akyol et al. 212 studied the effect
suggested that this phenomenon originates from parity-forbidden
of the oxide layer on the current-induced SOTs in perpendicularly
d-d transition of Cr3+ complexes, which displays broad linewidth
magnetized MgO-capped Hf/CoFeB and TaOx -capped Hf/CoFeB
due to strong vibronic coupling. Further, they fabricated het-
and found the significantly stronger torques for the former
erostructures formed by monolayer WSe2 and 2D magnetic CrI3
than the latter, which may be attributed to the different Rashba
and demonstrated the wide continuous tuning of the valley po-
like Hamiltonian arising from the difference in the electric
larization via the optical control of the CrI3 magnetization and
potential profiles across the oxide/ferromagnet interfaces, as
valley Zeeman splitting. 209 The WSe2 photoluminescence inten-
well as possible structural and oxidation differences in the
sity is dominated by the relative alignment between photoexcited
underlying CoFeB and Hf layers. Liu et al. 213 investigated the
spins in WSe2 with the CrI3 magnetization due to the ultrafast
effects of electrostatic gating on the current-induced phenomena

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in ultrathin ferromagnet/heavy-metal heterostructures and field-stabilized skyrmions in Fe3 GeTe3 nanoflakes (20 nm thick)
demonstrated that spin current produced by the spin Hall at cryogenic temperature using advanced magnetic electron mi-
effect plays the dominant role for current-induced phenomena, croscopy. Their further first principles calculations revealed a fi-
while the interfacial Rashba effect also provides a considerable nite interfacial DMIs in the Te/Fe3 Ge/Te slabs that determines
contribution to the current-induced torque. Ando et al. 214 the spin chirality in Fe3 GeTe2 . Using cryo-Lorentz transmission
reported that incorporating oxygen into Pt turns the heavy metal electron microscopy, Han et al. 228 found the topologically non-
into an electrically insulating generator of the SOTs, which leads trivial skyrmionic bubbles with homochirality in exfoliated insu-
to the electrical switching of perpendicular magnetization in a lating 2D vdW Cr2 Ge2 Te6 , which originates from the competition
ferrimagnet and can be controlled through voltage-driven oxygen between dipolar interactions and uniaxial magnetic anisotropy.
migration. Wang et al. 215 realized the switchable magnetization Yuan et al. 229 investigated the intrinsic magnetic skyrmions in the
of few-layered Fe3 GeTe2 /Pt through the SOTs originating from monolayer Janus TMDs, i.e., MnSTe, MnSeTe, VSeTe, and MnSSe.
the current in the Pt layer, which is quantitatively characterized Due to the out-of-plane geometric asymmetry and strong SOC,
by their harmonic measurements. Alghamdi et al. 216 exfoliated monolayer MnSTe and MnSeTe can stabilize a sub-50 nm intrinsic
Fe3 GeTe2 flakes (∼15-23 nm) and sputtered 5 nm Pt onto the skyrmions without magnetic field, while monolayer VSeTe with

Nanoscale Accepted Manuscript

atomically flat surface forming Fe3 GeTe3 /Pt heterostructures. in-plane easy axis forms magnetic domain rather than skyrmions.
Published on 16 December 2019. Downloaded on 1/2/2020 [Link] PM.

They further found that the spin current generated in Pt presents Combining the ferromagnetic monolayer (CrX3 , X = Cl, Br, and I)
a damping-like SOTs on Fe3 GeTe2 magnetization with high with antiferromagnetic substrate (MnPX3 , X = S, Se, Te), Tong
switching efficiency, which is comparable with that of the het- et al. realized the moiré skyrmions in 2D magnets originating
erostructures containing conventional 3D ferromagnetic metals from the moiré pattern vdW heterostructures. 230 They found that
and much larger than that of heterostructures containing 3D skyrmion vorticity and location in the moiré can be switched by
ferrimagnetic insulators. magnetic field in the strong interlayer coupling situation, while
the metastable skyrmion excitations can be moved between the
ordered moiré trapping sites by current pulses for the weak inter-
4.9 Skyrmion in 2D magnet
layer coupling case.
Magnetic skyrmions are one special kind of topological spin tex-
tures that can be stabilized by Dzyaloshinskii-Moriya interac-
5 Ferromagnetic 2D devices
tions (DMIs). 217 Skyrmions have attracted intense interest dur- Manipulating exchange interactions in magnetic heterostructures
ing the past decades for their promising potentials in spintron- has been proven to be an effective way to engineer functional
ics technology, such as energy-efficient logic and memory de- materials. 231 Thus the incorporation of magnetism with semicon-
vices. Early researches about skyrmions are focusing on the bulk ductor is particularly enticing for spintronics. The use of 2D ma-
materials (e.g., MnSi, FeCoSi, MnGe, FeGe etc), 218–220 the in- terials to form magnetic heterostructures has the advantage that
vestigations of atomic-scale skyrmions within the 2D limit have the proximity-induced exchange interaction, which is usually con-
emerged in the recent years. Heinze et al. 221 observed magnetic sidered as a perturbation for bulk materials, can fundamentally
skyrmion in 2D ultrathin Fe/Ir(111) bilayers at low temperature alter the electronic structure of the 2D system due to their atomic
(T=11±2K), which was attributed to the significant interfacial thickness. Compared to the approach to interfacing 2D materials
DMIs. Yang et al. 222 verified the physical mechanisms of DMIs with 3D magnets, a vdW heterostructure has the following ad-
in bilayers Co/Pt using first principles calculations. Soumya- vantages: (i) No need to consider lattice mismatch, thus almost
narayanan et al. 223 realized the tunable room-temperature mag- keeping the pristine layered structure without chemical modifi-
netic skyrmions in Ir/Fe/Co/Pt multilayers by varying the Fe/Co cation and interfacial damage, which is necessary to study the
composition that influences the magnetic interactions thus gov- optimal interactions between different layers. (ii) The interlayer
erning skyrmion formation. Boulle et al. 224 also reported the ob- twisting angle and stacking order can be treated as new knobs
servation of stable skyrmions in sputtered ultrathin Pt/Co/MgO to study and engineer the magnetic characteristics (e.g., spin tex-
nanostructures at room temperature without magnetic field. Most tures). (iii) The flexibility of the layered structure enable control-
recently, the successful synthesis of a variety of 2D intrinsic vdW ling the stacking process and facilitating the formation of vdW
magnets stimulates the research for finding 2D hosts with intrin- heterostructures with a diversity of 2D ferromagnets. Therefore,
sic DMIs and skyrmions. Park et al. 225 reported the experimental ferromagnetic 2D heterostructures provide a convenient platform
observation of magnetic skyrmions in Fe3 GeTe2 vdW ferromag- to explore the magnetism related condensed matter physics and
net flake and demonstrated that the skyrmion crystal state is ho- make it possible for realizing the application of spintronics.
mochiral and can be generated by both dynamically using current Xu et al. 179 realized a multiple-spin-filter magnetic tunnel
pulses and statically using magnetic field-cooling process. On junctions by using the CrI3 as spin-filter tunnel barrier and
the basis of first principle calculations, they further unveiled its reached a record of enhanced magnetoresistance for four-layer
possible origin of DMIs. Wu et al. 226 demonstrated that a large junction structures [Fig. 8(a)]. Further, they realized effec-
interfacial DMIs at the 1T’-WTe2 /Fe3 GeTe2 interface could be in- tive control of the spin and valley pseudo-spin in CrI3 /WSe2
duced due to the strong SOC in 1T’-WTe2 , which breaks the in- ferromagnetic heterostructure via flipping the magnetization of
version symmetry and stabilizes Néel-type skyrmions in the vdW CrI3 . 141,231 Ultrafast spin-dependent charge hopping across the
heterostructures. Wang et al. 227 reported the Néel-type, zero- heterostructure interface indicates the strong dependence of the

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relative alignment between photoexcited spin and magnetiza- nipulating the robust magnetic ordering at ambient temperatures,
tion. Wu et al. 232 demonstrated that the topological surface understanding the origin 2D ferromagnetism thoroughly, intro-
states of Bi2 Se3 can be persisted and magnetized via forming the ducing quantum band topology into high-temperature 2D ferro-
CrI3 /Bi2 Se3 /CrI3 heterostructure. Mak et al. 131 fabricated dual- magnets, and integrating the 2D FM-based device into modern
gate graphene/BN/CrI3 field-effect device and realized the effec- electronic processes. The recent high-throughput prediction of
tive control of magnetism in bilayer antiferromagnetic CrI3 by novel 2D materials 236,236 and topological materials 237–239 offers
tuning gate voltage. Zhang et al. 133 developed a device fabrica- a new arena for designing new 2D ferromagnetic materials to
tion technique using isolated Fe3 GeTe2 monolayers from the lay- overcome the challenges in practical application of 2D FM’s for
ered bulk material, realizing the ferromagnetic transition at room information technologies.
temperature. Controlled fabrication methods enable the tailoring
of layered structures with specific spin-dependent transport char- Conflicts of interest
acteristics, which usually combine a variety of 2D structures rang- The authors have no existing conflicts to declare.
ing from conductor and superconductor to insulator in respec-
tive of the conductivity. The rise of ferromagnetic and antiferro- Acknowledgements

Nanoscale Accepted Manuscript

magnetic insulators with magnetic order (e.g., CrI3 ) enriches the
Published on 16 December 2019. Downloaded on 1/2/2020 [Link] PM.

family of 2D functional materials. Recetnly, incorporating atomic The research was supported by the National Natural Sci-
thin layered CrI3 into vdW devices has been realized. 141 Benefit ence Foundation of China (Grant No. 11804230, 11774239,
from these findings, the 2D spin-dependent transport device–spin 61827815, 61805147, 61435010, and 61675135), the Science
valve–with adjustable conductivity via manipulating the relative and Technology Innovation Commission of Shenzhen (Grant
orientation of two ferromagnetic electrodes emerges. Tombros No. KQTD2015032416270385, KQTD20170810105439418,
et al. reported the lateral graphene spin valve with a relative long JCYJ20170818093035338, JCYJ20170412110137562,
spin relaxation length over micrometre-scale distances (1.5-2 ZDSYS201707271554071, GJHZ20180413181813768),
µm) at room temperature. 233 Jarillo-Herrero et al. demonstrated the Science and Technology Development Fund (Grant
a double spinfilter in graphite/CrI3 /graphite junctions where the No. 007/2017/A1 and 132/2017/A3), Macao SAR, China,
CrI3 tunnel barrier and the decoupled magnetic layers can be and the National Key R&D Program of China (Grant No.
treated as a magnetic memory bit for data storage [Fig. 8(b)]. 201 2016YFB0700700).
Furthermore, they realized the collective magnetic behavior (i.e.,
magnons) in CrI3 . Taking advantage of the spin-orbit torques de-
Notes and references
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The recent advances for 2D ferromagnets are reviewed, including materials synthesis,
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ferromagnetism modulation, physical properties, and potential device applications.

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 Published on 16 December 2019. Downloaded on 1/2/2020 [Link] PM.
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