Journal of Physics and Chemistry of Solids 167 (2022) 110754

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Journal of Physics and Chemistry of Solids

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Lateral magnetic tunnel junctions with a heterointerface-induced half-

metallic electrode
Yanxing Song a, *, Changchun Chai a, Qingyang Fan b, **, Wei Zhang a, Yintang Yang a
a
State Key Discipline Laboratory of Wide BandGap Semiconductor Technology, School of Microelectronics, Xidian University, Xi’an, People’s Republic of China
b
School of Information and Control Engineering, Xi’an University of Architecture and Technology, Xi’an, People’s Republic of China

A R T I C L E I N F O A B S T R A C T

Keywords: The electronic properties of monolayer MnGeSe3 and MnGeSe3/CrI3 heterostructures were investigated by
Half-metallicity density functional theory (DFT) calculations. In the MnGeSe3/CrI3 heterostructure, the half-metal MnGeSe3 can
CrI3/MnGeSe3 heterostructure induce the half-metallic properties of CrI3 by charge transfer. Based on the charge transfer effect, we designed
Magnetic tunnel junctions
lateral magnetic tunnel junctions (MTJs) in which MnGeSe3 attaches to the bottom of the detached CrI3 crystals.
Carrier transfer
This model can form half-metallic-CrI3/insulating-CrI3/half-metallic-CrI3 MTJs, thereby avoiding the loss of half-
metallic properties caused by defects and lattice distortion at the interface of traditional half-metallic MTJs.
According to the extension length of the CrI3 layer, they can be divided into heteroelectrode MTJs and MnGeSe3-
electrode MTJs. Half-metallic electrode MTJs are famous for their ultrahigh tunnel magnetoresistance (TMR),
and the ability to maintain a stable TMR under bias has become the other significant target of half-metal MTJs.
We find that the half-metallic gap of the electrode material can affect the threshold bias voltage in antiparallel
configuration (APC) when opening and closing. The larger the half-metallic gap is, the larger the bias voltage
required to generate the tunneling current, and correspondingly, the better its ability to maintain a high TMR.
Therefore, it is imperative to find two-dimensional half-metallic materials with large half-metallic gaps. Our
results provide a new idea for designing half-metallic electrode MTJs and provide a new understanding of the
mechanism of half-metallic electrode MTJs under bias.

1. Introduction atom) and large spin exchange splitting [3]. Gong et al. successfully
exfoliated FM CrGeTe3 atom layers [1]. Beginning with CrGeTe3,
Since CrI3 and Cr2Ge2Te6 were successfully prepared in 2017, self- transition-metal trichalcogen has become one of the most popular 2D
magnetization in two-dimensional (2D) materials has broken through ferromagnetic systems. CrSnTe3 [4], CrGaSe3, CrGaTe3 [5], CrGeS3 [6]
the limitation of Mermin-Wagner theory and emerged in the field of and VSeTe [7,8] monolayers are predicted to be candidates for FMSs. In
vision of researchers [1,2]. The 2D ferromagnetic materials have a addition, comprehensive calculations of TMAX3 (TM = V, Cr, Mn, Fe,
long-range magnetic order in the monolayer, and the interlayer is bound Co, Ni; A = Si, Ge, Sn; X = S, Se, Te) were performed by Chittari et al.,
by van der Waals (vdW) forces, which easily stack with other who found that most transition-metal trichalcogens were magnetically
two-dimensional materials to form heterojunctions. Two-dimensional ordered [9]. As the other star in two-dimensional magnetic materials,
magnetic materials provide new possibilities for the fabrication of new single-layer chromium trihalides CrX3 (X = F, Cl, Br, I) have been proven
electronic devices with high information storage density, ultrafast to be stable and ferromagnetic, and these CrX3 materials retain their
response and high integration. Benefitting from the efforts of re­ intrinsic magnetism under elastic tensile strain; additionally, the
searchers, a series of 2D magnetic materials have been discovered. FM-AFM phase transitions of CrCl3 CrBr3 and CrI3 occur at 2.5%, 4.1%
CrGeTe3 and CrI3 are prototype materials for their respective crystal and 5.7% strains, respectively [10–13]. Moreover, FeI3 with
classes. By using the ab initio calculation method, Yang’s group first strain-controllable high Curie temperature and magnetic crystal
estimated CrSiTe3 and CrGeTe3 monolayers to be ferromagnetic semi­ anisotropy have been reported by Guan et al. [14].
conductors (FMSs) with a large local magnetic moment (~3.5μ per Cr Notably, vdW spintronic devices have received extensive attention

* Corresponding author.
** Corresponding author.
E-mail addresses: syx739686768@163.com (Y. Song), qyfan_xidian@163.com (Q. Fan).

https://doi.org/10.1016/j.jpcs.2022.110754
Received 10 February 2022; Received in revised form 31 March 2022; Accepted 21 April 2022
Available online 26 April 2022
0022-3697/© 2022 Elsevier Ltd. All rights reserved.
Y. Song et al. Journal of Physics and Chemistry of Solids 167 (2022) 110754

based on the easy assembly of two-dimensional vdW crystals. A large monolayer MnGeSe3 to be consistent with HSE06 calculations. A vac­
number of studies have shown that layered CrI3 and its group are po­ uum space of 20 Å in the normal direction to the structures is used to
tential materials for vdW tunnel junction insulation [15–25]. When the avoid the interaction between the neighboring cells. For monolayer
graphene contacts attached to the same side of the stripped CrI3, the crystals and vertical devices, a 16 × 16 × 1 k-point mesh is used for
device exhibited the characteristics of an effective transistor, and when integration over the first Brillouin zone in the structural relaxation,
the graphene contacts attached to both sides of the CrI3, the device self-consistent field and electronic properties calculations. For lateral
exhibited a tunneling reluctance of 10000%. Due to ordered interlam­ devices, the k-points mesh is set to 16 × 1 × 1. Moreover, 64 × 64 × 1
inar antiferromagnetic coupling, the TMR of Graphene/n⋅CrI3/­ and 256 × 1 × 1 Monkhorst–Pack k-points are used for calculating the
Graphene tunnel junction increases with the increase in the number of local density of states, scatter states and transmission coefficients of
CrI3 layers [15–18]. A first-principles calculation reveals that there is an vertical and lateral MTJs, respectively. The TMR ratio is defined as
odd-even effect between the TMR and CrI3 layers in CrI3/h-BN/n⋅CrI3; TMR= (IPC-IAPC)/IAPC, where IPC and IAPC are the total current for the
when the CrI3 layer number is odd, the TMR of the device is larger [19]. parallel configuration (PC) and antiparallel configuration (APC) of
Spin polarization is an important factor in the performance of magnetic magnetizations of two electrodes, respectively. At zero bias when all
tunnel junctions. A higher spin polarization usually means a higher currents vanish, we use the transmission coefficient at the Fermi level to
TMR. Half-metals only have one spin channel at the Fermi level, calculate TMR.
resulting in nearly 100% spin polarization and making them a
high-quality electrode material. Although half-metals have large spin 2. Results and discussion
polarization, their interfacial states weaken the interfacial spin polari­
zation and thus reduce the TMR ratio in traditional half-metallic MTJs Monolayer CrI3 and MnGeSe3 have the same space group P-31m.
[26–28]. Therefore, layered half-metal appears in the vision of re­ Fig. 1(a and b) shows the top view and front view of monolayer CrI3. The
searchers as a superior electrode material. At present, 2D vdW ferro­ transition metal chromium is located at the center of a slightly distorted
magnetic half-metals are mainly found in Mn alloys, such as ternary octahedron formed by six iodine atoms. Fig. 1(c and d) shows the top
alloys MnXY4 (X = As, Sb; Y= S, Se) [29,30] and binary alloys Mn3X4 (X view and front view of monolayer MnGeSe3. A manganese atom is
= Te, S, Se) and MnX (X = P, As) [31,32]. Otherwise, 2D iron dihalides located at the center of a slightly distorted octahedron formed by six
are also found to have intrinsic half-metallic properties [33]. Doping and selenium atoms. In contrast, each of the two germanium atoms in the
carrier transfer of magnetic semiconductors can also induce unit cell is only threefold coordinated to the selenium atoms. Fig. 1(e
half-metallic properties [23,34–39]. At present, reports of 2D and f) shows the vdW heterostructure of CrI3 and MnGeSe3. The red
half-metallic MTJs are few. Li et al. found that lithium doping can induce dotted lines represent the primitive lattice in the hexagonal unit cell, and
half-metallic properties of CrI3, and an ultrahigh TMR is found in the the blue dotted lines represent the non-primitive lattice mutually
lateral Li0⋅5CrI3/CrI3/Li0⋅5CrI3 tunnel junction with the half-metal elec­ perpendicular directions in the rectangular unit cell. The vacuum is not
trode [23]. It is extremely difficult to form lateral presented in figures. As shown in Table 1, the optimized lattice pa­
half-metal/insulator/half-metal heterojunctions by doping; therefore, rameters a of CrI3 and MnGeSe3 are 6.868 Å and 6.300 Å, respectively. It
we constructed a new half-metallic electrode MTJ type based on the can be seen that the calculated lattice parameter of CrI3 is in excellent
charge transfer-induced half-metallic properties. agreement with the experimental result. Because of the little difference
In this work, we first studied the electronic properties of single-layer of the lattice parameters, the same amount of cells of CrI3 and MnGeSe3
MnGeSe3 and MnGeSe3/CrI3 heterostructures. From the band structure are used in the heterostructure. The lattice parameter a of the CrI3/
calculations, Monolayer MnGeSe3 is found to be an intrinsic ferromag­ MnGeSe3 heterostructure is 6.5 Å. The calculated lattice mismatch of the
netic half-metal; more interestingly, CrI3 in the heterostructure is two monolayers in the CrI3/MnGeSe3 heterostructure is 4.6%, which is
induced to be half-metallic because of charge transfer. Due to the half- acceptable in the theoretical study of the 2D heterostructure. Phonon
metallic properties of monolayer MnGeSe3 and MnGeSe3/CrI3 hetero­ dispersions of monolayer MnGeSe3 are shown in Fig. 2(a), and the
structures, the spin polarizations of the electrodes are all close to 100% phonon spectrum without virtual frequency proves the dynamic stability
when the above structures are adopted. Next, one vertical MTJ and two of MnGeSe3. Elastic constants of monolayer CrI3 and MnGeSe3 are also
lateral MTJs are designed, and the electron transport properties of MTJs given in Table 1, the mechanical stability of monolayer CrI3 and
are investigated using the nonequilibrium Green’s function-density MnGeSe3 is verified after bringing the elastic constants in to the
functional theory method (NEGF-DFT). constraint equations: C11 > 0, C211 > C212 . To ascertain the thermody­
namic stability, the interface binding energy of the heterostructure was
1.1. Ab initio calculation details calculated at different distances of separation between the individual
constituent monolayers, as shown in Fig. 2(b), using the following
Structural relaxation and HSE06 calculations were carried out using formula:
the Vienna ab initio simulation package (VASP) [40–43]. The
Eb = Ehetero. − ECrI3 − EMnGeSe3
plane-wave basis set is based on the projector augmented wave (PAW)
pseudopotential with a cutoff energy of 500 eV. Nonequilibrium spin
where Ehetero., ECrI3 and EMnGeSe3 are the total energies of the hetero­
polarized quantum transport calculations were performed by the
bilayer, CrI3 and MnGeSe3 monolayer, respectively. The binding en­
Nanodcal package based on real-space DFT combined with the
ergies of the CrI3/MnGeSe3 heterostructure are found to reach − 14.67
nonequilibrium Greens function formalism [44,45]. The convergence
meV/Å2 at the vdW minimum, implying that the process of hetero­
criteria for energy and force are set to 10− 5 eV and 0.001 eV A− 1.
bilayer formation is exothermic. As shown in Fig. 2(b), the interlayer
High-symmetry k points M and K for hexagonal lattice are define as (0
spacing of the heterostructure system in minimum energy is 3.37 Å.
0.5 0) and (0.333 0.333 0), respectively. The exchange correlation in­
To evaluate the magnetic ground state of single-layer CrI3 and
teractions are described by the generalized gradient approximation
MnGeSe3. Four possible different magnetic configurations are consid­
(GGA) of the Perdew–Burke–Ernzerhof (PBE) version [46]. To better
ered: Ferromagnetic state (FM), Néel antiferromagnetic state (n-AFM),
describe the influence of vdW interactions on crystal structure and
ZigZag antiferromagnetic state (z-AFM) and stripy antiferromagnetic
properties, DFT-D3 (BJ-damping) correction is adopted in the calcula­
state (s-AFM) [14]. The total energy of the four magnetic configurations
tions. In DFT + U calculations, we used Ueff values for transition metals
are given in Table 1. The results indicate that most stable magnetic state
suggested by the reported works [47,48]. As shown in Fig. S1, we have
is the FM state. This means that the monolayer MnGeSe3 is an intrinsic
also performed additional tests using other Ueff values from 1 to 5 eV,
ferromagnetic crystal. All structures with different magnetic
found that the adopted Ueff value correct the electronic properties of

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Y. Song et al. Journal of Physics and Chemistry of Solids 167 (2022) 110754

Fig. 1. Structures of monolayer CrI3 (a, b), monolayer MnGeSe3 (c, d) and their heterostructures (e, f). The red dotted line presents the primitive lattice in the
hexagonal unit cell, and the blue dotted line presents the mutually perpendicular directions in the rectangular unit cell.

Table 1
The lattice parameter (Å), elastic constants (N/m), total energy per unit cell with different magnetic configuration (eV) and Curie temperature (K) of monolayer CrI3
and MnGeSe3.
a C11 C12 EFM En-AFM Ez-AFM Es-AFM TNN
C

CrI3 6.868 27.7 6.9 − 67.336 − 67.271 − 67.264 − 67.295 44.1

MnGeSe3 6.300 62.8 20.9 − 107.030 − 106.884 − 106.753 − 106.979 99.2
CrI3 (Exp) 6.867 [12] 45 [11]

Fig. 2. (a) Phonon dispersions of monolayer MnGeSe3. (b) Variation in the binding energy per unit of interfacial area of the MnGeSe3/CrI3 heterobilayers along with
the interlayer distance.

configurations are fully optimized. Considering only the first-nearest past few years, and monolayer CrI3 is an indirect semiconductor with a
neighbors, the Curie temperature (TC) of monolayer CrI3 and MnGeSe3 1.53 eV gap10. In this work, the electronic properties of single-layer
are estimated by Monte Carlo method. In this work, the Ising Hamilto­ MnGeSe3 are investigated, and the properties of CrI3 are referred to in
nian Hspin = -Σ<i, j>J → si → s j was adopted, where J represents the the reported work. The band structures and density of states of the
nearest-neighbor exchange integral, → s ij represents the spin moment at HSE06, PBE and PBE + U band structures are shown in Fig. 3. Notably,
the metal atom site labeled by i, j. We take semi-integer values S = 3/2 the spin-up bands cross the Fermi level, while the spin-down channel
μB for spin magnitudes [9]. In Néel model, exchange parameter can be acts as a semiconductor, indicating that it is an intrinsic half-metallic
explicitly expressed as: J = (En-AFM-EFM)/12S2. Based on the above material with a 100% spin-polarization ratio. The HSE06 density of
Hamiltonian, Monte Carlo simulations were performed on a 32 × 32 states (DOS) further confirms its half-metallic property that spin-down
honeycomb lattice with 480000 step iterations for each temperature to electrons have no occupation state near the Fermi energy. The HSE06
investigate the temperature dependence of magnetization. The transi­ half-metallic gap for single-layer MnGeSe3 is 0.88 eV, and the spin gap
tion temperature between magnetic order and magnetic disorder is for the semiconducting channel is 1.46 eV. Half-metallic gap is defined
defined as Curie temperature. As shown in Table 1, the TC of monolayer as the difference between Fermi level and the valence band maximum of
CrI3 and MnGeSe3 are 44.1 K and 99.2 K, respectively. The corre­ minority spin subband. The spin gap presents the gap of minority spin
sponding experimental Curie temperatures of monolayer CrI3 is 45 K subband. The half-metallic gap and spin gap influence the ability of the
[11]. Our results are in great agreement with the experiment, and the half-metal to resist thermal fluctuations. To achieve great prospects for
monolayer MnGeSe3 shows a higher Curie temperature than that of CrI3. half-metallics in spintronic devices, wide half-metallic gaps and spin
The electronic properties of CrI3 have been researched widely in the gaps are extremely important. The contribution of the MnGeSe3 spin-up

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Y. Song et al. Journal of Physics and Chemistry of Solids 167 (2022) 110754

Fig. 3. (a)–(c) Band structure and PDOS of MnGeSe3: (a) HSE06, (b) PBE, and (c) PBE + U. (d)–(e) Band structure and Atom-projected density of states of MnGeSe3/
CrI3 heterostructure: (d) HSE06, (e) PBE, and (f) PBE + U. Black and red lines in the band structure present spin up electrons and spin down electrons, respectively.
The Fermi level is set to zero.

DOS near the Fermi energy mainly comes from Mn-d electrons and Se-p electrons transfer from the MnGeSe3 layer to the CrI3 layer. Similarly,
electrons, the Mn – Se – Mn bond angle in monolayer MnGeSe3 is the CrI3 layer was theoretically reported to switch to the FM half-metal
89.815◦ . Based on the Goodenough-Anderson rules, this shows a long- in Li0⋅5CrI3/CrI3, CrI3/CrGeTe3, graphene/CrI3 and CrI3/Sc2CO2 vdW
range ferromagnetic superexchange interaction and Se atoms act as heterostructures due to the shift of electrons from layer to layer32-35.
the bridge in superexchange [49,50]. For contrast and complement, the Based on the interlayer charge transfer effect in vdW heterojunctions, a
band structures and DOS were also calculated with the PBE and PBE + U half-metal/insulator/half-metal lateral MTJ can be formed by attaching
methods. As shown in Fig. 3(b and c), the results of PBE + U are monolayer CrI3 to the cut MnGeSe3. In this work, we further studied the
consistent with the above HSE06 results, i.e., they are FM half metals. quantum transport of this system.
The PBE + U half-metallic gap and spin gap are decreased to 0.55 eV and As shown in Fig. 4(a), the vertical MTJ is based on the vdW heter­
0.91 eV, respectively. However, the PBE results are different for the ostructure MnGeSe3/half-metal CrI3/MnGeSe3, in which monolayer CrI3
HSE06 and PBE + U results, indicating that monolayer MnGeSe3 is a is sandwiched between two monolayer MnGeSe3. As shown in Fig. 4(b),
conductor without half-metal properties. Therefore, in the subsequent the lateral MTJ heterostructure electrode is based on the lateral struc­
transport calculations, we adopted the PBE + U method instead of pure ture heterostructure/insulator CrI3/heterostructure, in which mono­
PBE. Moreover, the band structure of the CrI3/MnGeSe3 heterostructure layer CrI3 is overlaid with MnGeSe3 that has been cut open. As shown in
is calculated by the HSE06, PBE + U and PBE method. As shown in Fig. 3 Fig. 4(c), the MnGeSe3 electrode lateral MTJ is based on the lateral
(d and e), the CrI3/MnGeSe3 heterostructure is also a half-metal struc­ structure MnGeSe3/heterostructure/insulator CrI3/heterostructure/
ture, and the HSE06 half-metallic gap and spin gap are 0.16 eV and 1.44 MnGeSe3, in which the CrI3 nanoribbon is attached to the MnGeSe3
eV, respectively. Interestingly, the half-metallic properties of the het­ contact by vdW interactions. Regarding lateral MTJs, the distance be­
erostructure are not only derived from the MnGeSe3 layer, in which a tween two MnGeSe3 contacts is 11.4 Å, indicating that the width of the
subband contributed by CrI3 appears near the Fermi level. The Bader barrier is 11.4 Å. The local density of states (LDOS) of the majority
charge analysis for the heterostructure shows that approximately 0.059 carrier of MTJs is plotted under the structure figure in Fig. 4. The local

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Y. Song et al. Journal of Physics and Chemistry of Solids 167 (2022) 110754

Fig. 4. Side view and local density of states of the vertical MTJ (a), lateral heteroelectrode MTJ (b) and lateral MnGeSe3-electrode MTJ (c). The vertical MTJ is
periodic in the x and y directions. The lateral MTJs are periodic in the x direction, and the vacuum is below MnGeSe3 and above CrI3 along the z direction. The
current travels in the y direction. Local density of states (LDOS) are shown under the corresponding structures, which the red color presents a larger density of states
and blue is the opposite.

density of states present the density of states projecting in real space. As circles), we found that the spin-up electrons dominate the current
shown in Fig. 4, the LDOS have been summed in x and y directions, and contribution for both PC and APC in the systems, which agrees with
the density of states along the z direction can be clearly observed. The electronic states near the Fermi level being occupied by spin-up elec­
Fermi energy is used as the zero of the energy scale. For lateral MTJs, trons. The CrI3 barrier is configured to ferromagnetism, which as same
CrI3 with a 0.7 eV gap plays the role of a barrier in lateral MTJs. The ends as the incoming electrode (Left electrode) whether in PC or APC state.
of the CrI3 barrier show metallic properties because of the influence of In the PC state, as shown in Fig. 5(a), electrons from the majority spin
the MnGeSe3 layer, and the actual thickness of the barrier is less than the subband (spin up) near the Fermi level enter the empty state of the
distance of MnGeSe3 contacts, which is 3.9 Å. The Fermi levels are minority spin subband (spin up) at the other electrode. Due to the half-
located at approximately 0.7 eV below the conduction band bottom of metallic property of the CrI3 layer in the heterostructure, the vertical
CrI3; hence, the MTJs work by direct tunneling as long as the bias MTJ is in the conductive state, so the current under bias voltage is much
voltage is less than this value. Our nonequilibrium transport calculations larger than that of the lateral MTJs. For lateral MTJs, compared with the
are performed below 0.6 V. Fig. 6(a) presents the calculated spin- heterostructure electrode MTJ, the tunneling current of the monolayer
polarized current currents of the MTJs versus a bias voltage up to 0.6 MnGeSe3 electrode MTJ is higher. To provide a more intuitive under­
V. For the vertical MTJ, it is obvious that the CrI3 layer in the vertical standing of the transport difference between the two lateral MTJs, the
MTJ is conductive, which agrees with the band structure calculations. real space scattering states of the heterostructure electrode MTJ and
Regarding the spin-polarized currents (curves with red squares and blue MnGeSe3 electrode MTJ were investigated. Fig. 7 shows the real space

Fig. 5. Band diagram of half-metallic electrode MTJs in Parallel configuration (a) and Antiparallel configuration (b).

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Y. Song et al. Journal of Physics and Chemistry of Solids 167 (2022) 110754

tunneling current of the lateral MnGeSe3 electrode MTJ increases

rapidly at approximately 0.5 V, while the lateral heteroelectrode MTJ
shows a large tunneling current beginning at a bias of 0.1 V. We find that
the value of the potential energy provided by the bias corresponds to the
half-metallic gap. The tunneling current of the magnetic tunnel junction
is the integral of the transmission coefficient in the bias window. To
further study the spin transport mechanism under APC, we calculated
the transmission coefficient before and after the half-metallic gap. In
Fig. 8, the transmission of lateral MTJs under 0.1 V, 0.3 V, 0.4 V, and 0.6
V are plotted. For the heteroelectrode MTJ, there is no transmission
coefficient in the bias window at a 0.1 V bias, while at a 0.3 V bias, the
transmission coefficient of the spin upward electron falls into the bias
window. Regarding the MnGeSe3 electrode MTJ, there is almost no
transmission coefficient in the bias window at biases of 0.1 V, 0.3 V and
0.4 V, and an obvious transmission coefficient peak only appears at a 0.6
When the potential difference between the two electrodes is less than the
half-metallic gap, that is, the potential energy provided by the potential
difference between the two electrodes to the minority carrier is less than
the energy difference between the minority carrier and the Fermi level,
the half-metallic electrode MTJs present a completely closed state in the
APC state. When the potential difference between electrodes is larger
than the half-metallic gap, the tunneling current increases rapidly.
Although the transport mechanism of the vertical MTJ is not based on
the tunneling effect, the vertical MTJ and lateral MnGeSe3 electrode
MTJ have similar I–V curves because of the same electrode material; that
is, when the bias voltage is less than a half-metallic gap, there is almost
no conduction current, and the current increases rapidly when the bias is
greater than a half-metallic gap. The electron transport properties of the
half-metallic MTJs at APC are mainly affected by the half-metallic gap of
the electrode materials.
Fig. 6(b) shows the calculated TMR versus bias up to 0.6 V of the
three types of MTJs. The vertical MTJ and lateral MnGeSe3-electrode
MTJ maintain a high TMR at a low bias voltage and decay rapidly when
the bias voltage is greater than 0.5 V. The TMR of the lateral hetero­
Fig. 6. (a) Current-voltage curve of the MTJs in PC and APC under bias. (b) electrode MTJ decays rapidly with increasing bias voltage and remains
TMRs of the MTJs versus bias.
oscillating at low values. The TMR under bias voltage is mainly affected
by the APC current, so the half-metallic gap is the key factor affecting the
scattering states of the two lateral MTJs at Fermi energy Ef. Four TMR of half-metallic electrode MTJs. A higher half-metallic gap can
transport channels are obtained, indicating that four subbands exist in maintain a high TMR at a higher bias voltage. In the equilibrium state,
the electrode along the transport direction, which also agrees with the the TMRs of the vertical MTJ, lateral heteroelectrode MTJ and lateral
calculated band structure of monolayer MnGeSe3 and the CrI3/MnGeSe3 MnGes3-electrode MTJ are 301515%, 70099% and 614848%, respec­
heterostructure in which their Fermi energy crosses four bands. The real tively. The TMRs at 0.6 V bias were 665%, 219% and 178%, respec­
space scattering states can clearly express the attenuation of the carrier tively. The large tunneling reluctance at low bias voltage indicates the
wave function in the central scattering region. Electrons are injected potential application prospect of half-metallic materials in magnetic
from the left electrode and attenuate rapidly as they cross the single- tunnel junction electrodes, and a sufficiently large half-metallic gap
layer CrI3 barrier. For the four transport channels, three of the four becomes the priority of searching for new two-dimensional half-metallic
transport channels of the MnGeSe3 electrode MTJ are open, while only materials.
one channel is open in the heterostructure electrode MTJ. For the het­
erostructure electrode MTJ, on the one hand, a scattered wave function 3. Conclusion
of the open channel only exists in the CrI3 layer of the right electrode. On
the other hand, only one of the four subbands near the Fermi level is Summarizing, we applied ab initio method to investigate the stabil­
mainly contributed by CrI3. Therefore, it can be inferred that the ity, magnetic and electronic properties of monolayer CrI3, MnGeSe3 and
tunneling effect of the heterostructure electrode MTJ mainly exists in their heterostructure. Intrinsic ferromagnetism is found in monolayer
the CrI3 layer, while the tunneling effect of the MnGeSe3 layer is sup­ MnGeSe3, and it shows a higher Curie temperature than monolayer CrI3.
pressed. The difference in the number of scattering channels is the main The HSE06 calculation indicates that monolayer MnGeSe3 is a half-
reason for the difference in tunneling current between the two lateral metal with a 0.88 eV half-metallic gap and a 1.75 eV spin gap. In the
MTJs in the PC state. DFT + U calculations, the values change to 0.55 eV and 0.91 eV,
In the APC state, as shown in Fig. 5(b), electrons from the majority respectively. Regarding the MnGeSe3/CrI3 heterostructure, HSE06 cal­
spin subband (spin up) near the Fermi level enter the empty state of the culations show that the CrI3 layer switches to the FM half-metal because
minority spin subband (spin up) at the other electrode. Since there is of electron transfer, and the half-metallic gap and spin gap of the het­
100% polarizability of half-metallic electrode at Fermi levels, the erostructure are 0.16 eV and 1.44 eV, respectively. To further investi­
tunneling probability of half-metal/barrier/half-metal MTJs at APC is gate the application of half-metals in MTJs, we designed one vertical
theoretically zero. Fig. 6 (a) shows the current-voltage curve of MTJs MTJ and two lateral MTJs. Regarding the lateral MTJs, monolayer CrI3
under bias. The conduction current of the three MTJs tends to be is attached to a layer of disconnected MnGeSe3. According to the
infinitesimal at low bias voltage, which is consistent with the electrical extension length of the CrI3 layer, it can be divided into heteroelectrode
properties of the half-metal electrode. As the bias increases, the MTJs and heteroelectrode MTJs. In the PC state, the tunneling effect

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Y. Song et al. Journal of Physics and Chemistry of Solids 167 (2022) 110754

Fig. 7. Real space scattering states of the lateral MnGeSe3 electrode MTJ and lateral heteroelectrode MTJ at Fermi energy Ef. All the figures share the same color bar.
Scattering states are eigen-states of the Hamiltonian of the open device structure. The real space scattering states gives the number of scattering states per unit space,
which is proportional to the conductance in that region. The left electrode is the incoming electrode.

only occurs in the CrI3 layer for the lateral heteroelectrode MTJ, so only junctions under bias voltage and provide a new direction for the
one of the four scattering channels is open. Compared to the lateral exploration of half metal electrode materials.
heteroelectrode MTJ, three channels of the lateral MnGeSe3 electrode
MTJ are open, which induces a higher tunneling current. In the APC Author statement
state, we found that the tunneling current is closely related to the half-
metallic gap of the electrode. When the potential difference between the Yanxing Song: Formal analysis, Investigation, Conceptualization,
two electrodes is less than a half-metallic gap, the tunneling probability Writing - review & editing. Changchun Chai: Funding acquisition,
of electrons approaches infinitesimal. The tunneling probability in­ Methodology. Qingyang Fan: Conceptualization, Investigation, Vali­
creases rapidly when the potential difference is greater than the half- dation. Wei Zhang: Investigation. Yintang Yang: Validation.
metallic gap. In the equilibrium state, the TMRs of the vertical MTJs,
lateral heteroelectrode MTJ and lateral MnGeSe3 electrode MTJ are
Declaration of competing Interest
301515%, 70099% and 614848%, respectively. The TMR at 0.6 V bias
are 665%, 219% and 178%, respectively. In this work, two feasible
The authors declare the following financial interests/personal re­
schemes of MTJs with half-metal electrodes were designed, and further
lationships which may be considered as potential competing interests:
study on the transport mechanism revealed the importance of half-
Fan Qingyang reports financial support was provided by National Nat­
metallic gaps on the transport properties of the APC state. These re­
ural Science Foundation of China. Chai changchun reports financial
sults provide a promising route for stable TMR magnetic tunneling
support was provided by National Natural Science Foundation of China.

7
Y. Song et al. Journal of Physics and Chemistry of Solids 167 (2022) 110754

Fig. 8. Transmission coefficient versus electron energy for (a) lateral heteroelectrode MTJ and (b) lateral MnGeSe3-electrode MTJ at different bias voltages: 0.1 V,
0.3 V, 0.4 V and 0.6 V. The bias window in each panel is between the two red vertical dashed-dotted lines, and the light red area shows the transmission coefficients
that contribute to the current.

Fan Qingyang reports financial support was provided by China Post­ [14] Z. Guan, S. Ni, 02-Strain-Controllable high Curie temperature and magnetic crystal
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doctoral Science Foundation.
Electronic. Materials. 3 (2021) 3147–3157.
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This work was supported by the National Natural Science Foundation [16] T. Song, X. Cai, M.W. Tu, X. Zhang, B. Huang, N.P. Wilson, K.L. Seyler, L. Zhu,
of China (No. 61974116); the National Natural Science Foundation of T. Taniguchi, K. Watanabe, M.A. McGuire, D.H. Cobden, D. Xiao, W. Yao, X. Xu,
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