Acta Materialia 259 (2023) 119257

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Acta Materialia
journal homepage: www.elsevier.com/locate/actamat

Magnetotransport, spin reorientation, and anomalous

ferrimagnetic-to-antiferromagnetic phase transition in epitaxial Mn2Sb
alloy thin films
Ting-Wei Chen a, b, Shiqi Liu b, Ying Zhang a, Fang Tang c, Jing-Shi Ying a, Shuang-Shuang Li a,
Lei Chen d, Fu-Sheng Luo e, Shu-Juan Zhang a, Yong Fang c, Shanming Ke d, Weiyao Zhao f, *,
Ren-Kui Zheng d, **
a
School of Materials Science and Engineering and Jiangxi Engineering Laboratory for Advanced Functional Thin Films, Nanchang University, Nanchang 330031, China
b
Key Laboratory of Spintronics Materials, Devices and Systems of Zhejiang Province, Hangzhou 311305, China
c
Jiangsu Laboratory of Advanced Functional Materials, Department of Physics, Changshu Institute of Technology, Changshu 215500, China
d
School of Physics and Materials Science, Guangzhou University, Guangzhou 510006, China
e
School of physics and electronic information, Gannan Normal University, China
f
Department of Materials Science and Engineering, Monash University, Clayton VIC 3800, Australia

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

Keywords: High-quality ferrimagnetic Mn2Sb epitaxial thin films have been successfully grown on SrTiO3 (001) single-
Mn2Sb film crystal substrates via systematically optimizing the growth parameters using molecular beam epitaxy. Magne­
Anomalous Hall effect totransport and magnetic measurements reveal that a spin reorientation transition occurs in the 260–150 K
Antiferromagnetic phase
region where the direction of spins rotates from out-of-plane to in-plane upon cooling, resulting in the ferri­
Magnetoresistance
magnetic(II) phase, followed by a giant magnetoresistance associated anomalous ferrimagnetic(II)-to-canted
Molecular beam epitaxy
antiferromagnetic (c-AFM) phase transition in the 150–115 K region, resulting in the c-AFM ground state,
both of which are completely absent and have yet not been previously observed in Mn2Sb bulk and thin films.
Temperature-dependent X-ray diffraction measurements reveal that the low-temperature c-AFM phase originates
from the contraction of the out-of-plane lattice constant c, which would increase the exchange interaction be­
tween neighbouring magnetic sublattices and thus stabilize the c-AFM phase. DFT calculations reveal that
substrate clamping is the cause of the unique c-axis contraction in Mn2Sb films. For the 24-nm films, there is
almost no out-of-plane magnetization in the ground state, but exists a weak in-plane remanent magnetization
(~0.4 μB/f.u.) and anomalous Hall effects, implying spin canting within the ab plane. With decreasing film
thickness from 64 to 8 nm, the out-of-plane saturation magnetization at 10 K increases by approximately 10
times, and for the 8-nm film, its saturation magnetization (4.8 μB/f.u.) is 2.8 times larger than that of Mn2Sb bulk
(~1.74 μB/f.u.), both of which are attributed to the interfacial strain effect. Our work demonstrates that Mn2Sb
films grown on perovskite oxide substrates show anomalous spin-charge-lattice coupling phenomena, which may
inspire more study of its basic properties and potential device applications.

1. Introduction
The realization of stable and sizeable anomalous Hall effects (AHE)
at room temperature is important to achieve better performance of
electronic and spintronic devices. [1,2] For ferromagnetic materials, the
anomalous Hall current is generated in proportion to the magnetization
below the magnetic ordering temperatures (Curie temperature, TC). [3,
4] Recently, giant AHE was reported in hexagonal Mn3X (X=Sn, Ge, Ga,
and Pt) compounds, which are antiferromagnets with a noncollinear
120◦ spin coupling between the Mn Kagome lattice within their ab
planes. Such a triangle antiferromagnetic (AFM) structure contains
geometrical frustration and induces noncolinear AFM coupling between
Mn moments. [5–7] Due to the Dzyaloshinskii-Moriya (DM) interaction,
weak net magnetic moments have been observed in these compounds

* Corresponding author.
** Corresponding author.
E-mail addresses: weiyao.zhao@monash.edu (W. Zhao), zrk@ustc.edu (R.-K. Zheng).

https://doi.org/10.1016/j.actamat.2023.119257
Received 1 August 2022; Received in revised form 10 July 2023; Accepted 14 August 2023
Available online 19 August 2023
1359-6454/© 2023 The Author(s). Published by Elsevier Ltd on behalf of Acta Materialia Inc. This is an open access article under the CC BY-NC-ND license
(http://creativecommons.org/licenses/by-nc-nd/4.0/).
T.-W. Chen et al.
below the Néel temperature (TN ≈ 420 K), however, DM interaction is
not responsible for their surprisingly large AHEs. [8–11] Instead, the
nonvanishing Berry phase was proposed to explain the observed giant
AHE in Mn3Sn and Mn3Ge. [8,12] With the presence of a strong
spin-orbit coupling, the application of a small magnetic field leads to the
realignment of magnetic domains below TN, thus changes the Hall re­
sistivity dramatically. [13,14] Another scenario of spin coupling in
magnetic materials is the ferrimagnetism (FIM) in which there are two
magnetic sublattices with unequal antiparallel spins, resulting in net
magnetic moments like a ferromagnet (FM). The ordering temperature
of many ferrimagnetic materials are higher than room temperature
including rare-earth transition-metal alloy [15] and rare-earth-free
metallics [16], which enables potential room-temperature applica­
tions. In recent years, ferrimagnetic materials are popular in the
research of spin-orbital torque (SOT), and are considered to support the
application of the high-performance SOT-magnetoresistive random ac­
cess memory (SOT-MRAM). [15] Moreover, ferrimagnets possess unique
properties, e.g., fast magnetic field-driven AFM spin dynamics at the
angular momentum compensation point, [17,18] due to the interaction
between magnetic sublattices.
Materials that show high temperature FM or FIM phase and low
temperature AFM phase are of great interest in recent years. These
materials include magnetic alloys such as MnP [19], FeRh [20–23],
Fe3Ga4 [24], Gd5Ge4 [25], Nd5Ge3 [26], CeFe2 [27], and Mn2Sb [28,29].
Among them, Mn2Sb is an interesting material that undergoes high
temperature FIM to low temperature AFM phase transition during which
multiple physical quantities couple mutually, resulting in interesting
phenomena.
Mn2Sb is a FIM material, which crystallizes in the Cu2Sb-type
centrosymmetric tetragonal lattice with P4/nmm space group (a = 4.08
Å and c = 6.56 Å), showing a paramagnetic-to-FIM transition at 550 K,
below which the spins of the two kinds of Mn atoms, namely Mn(I) and
Mn(II) [Fig. 1(a)], aligns antiferromagnetically along the c axis, how­
ever, with unequal magnetic moments. [30] Upon cooling, a spin reor­
ientation (SR) transition occurs at ~260 K, where the direction of spins
of both sublattices rotates to the ab plane. [31,32] This transition is
sensitive to element substitutions, e.g., Co, Cr, Cu, Zn, V at Mn site, or Bi,
Sn at Sb site, [33–45] which consequently modifies the magnetic phase
transition temperatures, [33–37] magnetic domain structures, [38]
magnetostriction, and inverse magnetostriction, [39–41] magnetore­
sistance (MR), [42] magnetocaloric effect, [43] and topological Hall
effect [44,45] of Mn2Sb. The multi-dimensional coupling and tunability
of magnetism and other physical properties provides a good platform to
investigate the competing interactions among the spin, charge, and
lattice degrees of freedom and explore its potential device applications.
Fig. 1. (a) Schematic illustration of the tetragonal crystal structure of Mn2Sb
with two kinds of Mn atoms [Mn(I) and Mn(II)] occupying different crystallo­
graphic positions. (b) Usual growth mode of Mn2Sb films along the [001] di­
rection using SrTiO3 (001) substrates. (c) Mn2Sb (101) film could also be grown
on SrTiO3 (001) substrates via the domain matching epitaxial growth mode
because the Mn2Sb (101) plane matches the SrTiO3 (001) plane quite well.
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Acta Materialia 259 (2023) 119257
The magnetic structure of Mn2Sb has been determined in previous
reports [30,46]. Schematic diagram of the AFM and FIM(II) magnetic
structure is shown in Figure S1, Supporting Information. Each magnetic
sublattice of Mn2Sb contains Mn(II)-Mn(I)-Mn(II) triple layers, as indi­
cated by the dotted blue squares. Within a magnetic sublattice, there is a
strong direct exchange interaction between the neighbouring Mn layers,
which induces the particular Mn(II)←Mn(I)→Mn(II)←, or Mn(II)→Mn
(I)←Mn(II)→ spin arrangement. Because the magnetic moments of Mn
(I) and Mn(II) are different, each magnetic sublattice has a net magnetic
moment. Whether the coupling between neighbouring magnetic sub­
lattices is FM or AFM depends on the indirect exchange via the Sb 5p
states.
The aforementioned phenomena of Mn2Sb are observed in its bulk
form in the last several decades. To realize device applications, a
comprehensive study of Mn2Sb thin films is highly desired. Unfortu­
nately, there are only several literatures that reported the properties of
Mn2Sb thin films grown on GaAs and Si substrates, [47–51] which may
probably be due to the high difficulty in growing high quality
single-phase Mn2Sb films because their phase purity and out-of-plane
orientation are highly sensitive to growth parameters of molecular
beam epitaxy (MBE) and have significant impact on the physical prop­
erties, for example, the parasitic MnSb impurity phase [51,52] has
stronger ferromagnetism than that of Mn2Sb phase. Therefore, precise
adjustment of growth parameters is highly required to prepare highly
(001)-oriented Mn2Sb films in order to eliminate the in-plane lattice
misalignment which usually results in the MnSb phase. The impurity
phase, orientation fault, and other obstacles, e.g., high saturated vapor
pressure of Sb and possible self-doping effect at the interface, [53] slows
the basic and device research progresses of the Mn2Sb family. It is noted
that the growth of Mn2Sb films on lattice matched oxide single-crystal
substrates is missing until now. Another critical problem during thin
film deposition process is the good lattice match between the Mn2Sb
(101) plane and perovskite (001) plane [e.g., SrTiO3 (STO)] [Fig. 1(c)],
easily resulting in mixed out-of-plane orientations of Mn2Sb (001)
[Fig. 1(b)] and Mn2Sb (101) [Fig. 1(c)] films. Therefore, the growth of
high-quality single phase Mn2Sb epitaxial films on perovskite oxide
substrates is highly challenging.
In this paper, we report the growth of high-quality single phase
Mn2Sb epitaxial films on perovskite STO (001) substrates via system­
atically optimizing the growth parameters using MBE. The magneto­
transport, anomalous Hall effect, and magnetic properties of the Mn2Sb
(001) epitaxial films have been systematically studied. The detailed
results and discussion are presented in the following sections.
2. Experimental section
2.1. Thin film growth
Mn2Sb films were grown on one-side polished (001)-oriented STO (a
= 3.905 Å) single-crystal substrates with a size of 5 × 5 × 0.5 mm3 using
MBE, equipped with high purity Mn (Alfa Aesar, 99.995%) and Sb (Alfa
Aesar, 99.9999%) sources. The size of the hollowed part of the mask is
4.4 × 4.4 mm2, resulting in an effective area of films is approximately
4.4 × 4.4 mm2. The flux ratio of the Mn and Sb sources at fixed tem­
peratures are calibrated by quartz crystal microbalance. The MBE sys­
tem is operated in ultrahigh vacuum with a background pressure less
than 1 × 10− 10 mbar. STO substrates were cleaned with acetone,
alcohol, and deionized water in sequence to remove impurities, dried
with high purity nitrogen gas and further cleaned by Ar-O2 plasma.
Before the growth of Mn2Sb films, STO substrates were heated to 500 ℃
for degassing and decreased to a growth temperature of TS=330 ◦ C and
stabilized for 20 min, followed by the growth of Mn2Sb films. After
optimizing the substrate temperature [Figure S2(a), Supporting Infor­
mation] and flux rates of Mn and Sb [Figure S2(b), S3, Supporting In­
formation], the growth rate of Mn2Sb films is determined to be ~2.67 Å/
min. Mn2Sb thin films with various thicknesses are employed to study
T.-W. Chen et al. Acta Materialia 259 (2023) 119257

the electronic transport and magnetic properties, of which 68 to 64-nm (ZFC) magnetization and magnetic hysteresis loops of Mn2Sb films
films are discussed here. were measured using a superconducting quantum interference device
(SQUID) (MPMS3, Quantum Design). Note that the diamagnetic signal
2.2. Structure and composition from STO substrates have been subtracted.

The crystallographic properties of Mn2Sb films were characterized
by X-ray reflectivity (XRR) and X-ray diffraction (XRD) rocking curve (ω
scan), θ− 2θ and φ scans at room temperature using a Rigaku SmartLab
X-ray diffractometer equipped with Cu Kα1 X-ray source (λ=1.5406 Å).
The low temperature XRD θ− 2θ scan measurements were conducted
after the Mn2Sb film was stabilized at each temperature for 5 min, using
a Bruker D8 X-ray diffractometer equipped with High-brilliance 6 KW
rotational Cu X-ray source (λ=1.5406 Å). The elemental mapping of Mn
and Sb elements were measured using an energy dispersive X-ray
spectroscopy (EDS) attachment (Ultim Max 65, Oxford Instruments)
installed on a FEI focused ion beam system (Thermo Fisher Scientific,
Scios2). The surface morphology of Mn2Sb films were measured via the
atomic force microscopy using a Cypher ES atomic force microscope
(Oxford Instruments Asylum Research Inc.).
2.4. Density functional theory (DFT) calculations
DFT calculations are performed using the projector-augmented wave
(PAW) pseudopotential and a plane-wave cut-off energy of 500 eV
implemented in the QUANTUM ESPRESSO Package [54,55] and
DS-PAW [56]. A Γ-centered Kmesh-Resolved Value of 0.03 (in Units of
2*π/Angstrom) is used to generate the k-points in the Brillouin zone. The
maximum force is less than 0.02 eV A-1 per atom, and the energy is
converged to within 10− 5 eV between two successive steps. Generalized
gradient approximation (GGA) [57] of the Perdew–Burke–Ernzerhof
(PBE) [58] form to the exchange–correlation functional is applied
throughout the theoretical calculation.
3. Results and discussion

2.3. Electronic and magnetic properties
The anomalous Hall effect and magnetotransport properties of
Mn2Sb films were measured using a physical property measurement
system (PPMS) (DynaCool-14, Quantum Design). The zero-field-cooled
XRR, XRD θ− 2θ, ω, and φ scan measurements were performed to
check the phase purity, out-of-plane and in-plane orientations, crystal­
linity, and thicknesses of the Mn2Sb films. As shown in Fig. 2(a), (00l) (l
= 1, 2, 3, 4) diffraction peaks of a 16-nm Mn2Sb film and two strong
(00l) (l = 1, 2) diffraction peaks of the STO substrate are observed using

Fig. 2. (a) XRD θ− 2θ scan pattern for a 16-nm Mn2Sb film grown on a SrTiO3 substrate. (b) XRD rocking curve taken on the Mn2Sb (002) diffraction peak. (c, d) XRD
φ-scan patterns taken on the Mn2Sb (101) and SrTiO3 (110) diffraction peaks, respectively. (e) Laue oscillation of the Mn2Sb (002) diffraction peak. (f) XRD reciprocal
space mapping around Mn2Sb (002) diffraction peak. (g) RHEED pattern of the Mn2Sb film. (h) XRR pattern of a 20-nm Mn2Sb film. The red curve is the fitting of the
data. (i, j) EDS elemental mapping of the Mn and Sb elements. (k) Elemental spectrum of a Mn2Sb film.

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T.-W. Chen et al. Acta Materialia 259 (2023) 119257

the θ− 2θ scan. There are no diffraction peaks contributed by impurity

phases, nor by other orientations of the Mn2Sb film, which indicates the
successful growth of single phase and c-axis oriented Mn2Sb films on
STO substrates. The XRD ω-scan measurements taken on the Mn2Sb
(002) diffraction peak yields a rocking curve with a full width at half
maximum (FWHM) of 0.1◦ [Fig. 2(b)]. This, together with the reciprocal
space mapping pattern around the Mn2Sb (002) diffraction peak [Fig. 2
(f)], reveals the excellent crystalline quality of the Mn2Sb film. The XRD
φ scans taken on the Mn2Sb (101) and STO (110) diffraction peaks yield
four-fold symmetrical diffraction peaks from the Mn2Sb film, occurring
at the same azimuthal angles as those of the STO substrate [Figs. 2(c, d)],
revealing the epitaxial growth of the Mn2Sb film on the STO substrate.
Another feature of the XRD pattern is the Laue oscillations on both sides
of Mn2Sb (002) diffraction peak [Fig. 2(e)], which originates from the
interference of reflected X-ray by the smooth film surface and film-
substrate interface, following the Bragg’s law [59]:
λ
d= (1)
2(Sinθm − Sinθn )

where θm and θn denote the angle of two adjacent Laue oscillation peaks,
λ is the wavelength of X-ray. A film thickness d~16 nm can be obtained
using Eq. (1). The smooth surface morphology of the Mn2Sb film is
visualized by the AFM image shown in Figure S4 (Supporting Informa­
tion), in which the root-mean-square roughness of a 5 × 5 μm2 area is
~0.3 nm. The sharp streaky RHEED pattern [Fig. 2(g)] further indicates
high crystalline quality and smooth surface of the film. The fitting of the
XRR oscillation pattern obtained from a thicker 20-nm Mn2Sb film
(growth time: 75 min) [Fig. 2(h)] yields a surface roughness ~0.7 nm
and mass density ~7.1 g/cm3, which is close to the theoretical value of
7.05 g/cm3. The elemental mapping via EDS were performed on the
surface of the 16-nm Mn2Sb film within a relatively large area. As shown
in [Figs. 2(i, j)], the Mn and Sb elements distribute uniformly within the
measured area, with an atomic ratio of Mn/Sb=1.96 [Fig. 2(k)], close to
that of stoichiometric Mn2Sb. All these results demonstrate that the
Mn2Sb (001) film is high quality.
Hall measurements were performed on the 16-nm Mn2Sb film at
various fixed temperatures. As shown in Fig. 3(a), AHE is observed at
temperatures ranging from 2 to 300 K. We firstly focus on the AHE at
300 K, where the saturated AH resistivity (ρAH ) is ~0.6 μΩ cm above ~1
T. The saturated ρAH increases slightly with cooling from 300 to 250 K
(~1.0 μΩ cm) and shows less temperature dependent behaviors upon
further cooling to 150 K [inset (I) of Fig. 3(a)]. From 150 to 100 K, the
saturated ρAH decreases, which suggests a decrease in the saturated
magnetization. The AHE curves above 50 K show “S”-like shape, with
negligible coercive effect. However, a significant change occurs at T =
25 K, where the AHE changes its sign and show roughly squared shape.
At T = 2 K, the AHE keeps similar shape as that of the 25-K one, however,
shows a larger saturation ρAH . To evaluate the AHE in the Mn2Sb film,
the anomalous Hall conductivity (σ AH) is calculated using:
/( ) density. As shown in Table S1 (Supporting Information), R0 decreases
σ AH = ρyz ρ2yx + ρ2xx (2)
where ρxx is the longitudinal resistivity extracted from the MR data
shown in Fig. 3(b). The saturated σAH is 8.5 Ω− 1 cm-1 at 300 K, which is
nearly three times larger than that of the Mn2Sb bulk. [46] |σ AH| at 300
K is comparable to the reported values of noncollinear Weyl antiferro­
magnet Mn3Sn (|σ zx| ~ 20 Ω− 1 cm− 1, |σ yx| ~ 30 Ω− 1 m− 1). [60] The
significantly large AHE in epitaxial Mn2Sb films at room temperature is
favorable for its potential applications in electronic devices. As shown in
Fig. 3(b), the MR effect for T ≤ 24 K and T ≥ 175 K is rather weak while
for 25 K ≤ T ≤ 150 K it is much significant, which are closely related to
the magnetic phase transitions that will be discussed in the following
sections.
Fig. 4(a) shows that ρAH and σ AH reach maximum values at ~200 and
~150 K, respectively, which are probably related to the magnetic phase
Fig. 3. (a) Anomalous Hall resistivity vs. the magnetic field B for the 16-nm
Mn2Sb film. Inset I: Enlarge view of the saturated region of the Hall re­
sistivity curves. Inset II: Hall resistivity vs. B at T = 2 and 25 K. (b) MR vs. B in
the 2–300 K region for the 16-nm Mn2Sb film. Inset: MR vs. B curves in the high
field region.
transitions of the Mn2Sb film. To study their relationships, we split the
total Hall resistivity into ordinary and anomalous parts using:
ρxy = ρH + ρAH = R0 Bz + RS 4π Mz (3)
where ρH is the ordinary Hall resistivity, R0 is the ordinary Hall coeffi­
cient, RS is the anomalous Hall coefficient, B is the magnetic flux density,
Mz is the magnetization. R0 is estimated by the linear fitting of the ρxy vs.
B curves in the high field region. R0 at 300 K is ~2.8 × 10− 12 Ω cm / Oe,
which is comparable to those of other magnetic alloy bulks and thin
films. [60] The ordinary Hall effect term in Eq. (3) describes the influ­
ence of external magnetic field on charge carriers, which follows R0 =
1/ne, where e is the charge of an electron and n is the charge carrier
with decreasing temperature from 300 K, implying an increase in the
carrier density. ρAH is obtained by subtracting the resistivity contributed
from the ordinary Hall effect. The magnetization Mz in Eq. (3) is ob­
tained from the magnetic hysteresis loops which are shown in Fig. 4(b).
Note that the diamagnetic background has been subtracted to obtain
these loops. The loops also show “S” shape with negligible coercive field,
which suggests the soft magnetic nature of the film [61]. The coercive
field increases at low temperatures, e.g., T = 10 and 20 K [Fig. 4(b)],
which is consistent with the AHE curves shown in Fig. 3(a). For the
16-nm Mn2Sb film with saturation magnetization (Msat) ~315 emu/cc at
300 K, one can obtain RS ≈ 1.0 × 10− 10 Ω cm / G, which is 2~3 orders
smaller than that of noncollinear Kagome antiferromagnets, [46,60] and
about 11~50 times larger than usual metal ferromagnets (cf. Fe: |RS| =
7.3 × 10− 12 Ω cm / G, Co: |RS| = 2.0 × 10− 12 Ω cm / G and Ni: |RS| = 9.1
× 10− 12 Ω cm / G). [62]

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T.-W. Chen et al.
Fig. 4. (a) Anomalous Hall resistivity and Anomalous Hall conductivity plotted
against temperature for the 16-nm Mn2Sb film. (b) Magnetic hysteresis loops
measured at various temperatures for the 16-nm Mn2Sb film. Inset: Enlarge
saturated region of the magnetic hysteresis loops.
Fig. 5(a) and 5(b) show the temperature dependence of the in-plane
and out-of-plane ZFC magnetization, longitudinal resistivity ρxx, and MR
for the 16-nm Mn2Sb film, respectively. At high temperatures (e.g., 300
K), the Mn2Sb film is in the FIM(I) state, where the two Mn sublattices
possess different moments along the [001] and [001] directions (see the
right inset of [Fig. 11(a)]. For the measurements of magnetization, the
magnetic fields of B = 200 and 500 Oe were applied along the out-of-
plane [001] [i.e., B⊥ab, lower inset of Fig. 5(a)] and [100] [B//ab,
upper inset of Fig. 5(a)] crystallographic directions of the Mn2Sb film,
respectively. At 350 K, sizeable magnetization values are obtained for
both measurement configurations, in which the out-of-plane magneti­
zation are slightly larger than that of the in-plane ones. Upon cooling,
two magnetic phase transitions occur, which are reflected by the vari­
ation of the magnetization with temperature. Specifically: 1) the SR
transition approximately between 260 K and 150 K, where the direction
of spins of each Mn sublattice rotates from out-of-plane to in-plane,
which causes an increase in the in-plane magnetization and a decrease
in the out-of-plane magnetization within this temperature region,
resulting in the FIM(II) phase [light green area in Fig. 5(a)], and 2) the
FIM(II)-to-canted AFM (c-AFM) phase transition between 150 K and 115
K [yellow area in Fig. 5(a)], where the in-plane magnetization shows
rapid decrease and the out-of-plane magnetization shows appreciable
decrease. Within this phase transition area, the competing FIM(II) and c-
AFM phases coexist, which may give rise to possible exchange bias ef­
fect, as has been observed in previous reports [63]. For B = 200 Oe, the
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Acta Materialia 259 (2023) 119257
Fig. 5. (a) Temperature dependence of the zero-field-cooled in-plane and out-
of-plane magnetization for the 16-nm Mn2Sb film. (b) Temperature dependence
of longitudinal resistivity and magnetoresistance (MR) in various magnetic
fields for the 16-nm Mn2Sb film.
out-of-plane magnetization at 10 K is basically zero while there is a net
in-plane magnetization of 0.56 μB/f.u., indicating that the direction of
spins is canted within the ab plane. Namely, the low-temperature phase
is the c-AFM phase. The FIM(II)-to-c-AFM phase transition is also re­
flected by the temperature dependent zero-field resistivity which in­
creases remarkably below 150 K [Fig. 5(b)], induced by increasing
magnetic disorder and related carrier scatterings during the phase
transition. It is noted that the c-AFM phase has yet not been reported in
the undoped Mn2Sb phase either in the form of film or bulk before. [64,
65] Another feature is that the transition temperature (TFIM(II)− c− AFM ) is
sensitive to external magnetic fields. As shown in Fig. 5(b), TFIM(II)− c− AFM
can be shifted from 155 to 75 K by applying a 14 T magnetic field,
indicating that the c-AFM phase is suppressed by the magnetic field. In
this magnetic phase transition region (75–155 K), the magnetic scat­
tering plays a dominant role to the MR behaviors, e.g., negative MR up
to ~45% [upper panel of Fig. 5(b)].
The resistivity of all Mn2Sb films (8–64 nm) has been measured with
field cooling and field warming modes to verify whether the FIM(II)-to-
c-AFM phase transition is a first-order phase transition or not. Fig. 6
shows the temperature dependence of the resistivity in magnetic fields
of B = 0, 1, 5, 9, 14 T, with the direction of B perpendicular and parallel
to the film plane, respectively. In Figs. 6(c), 6(d), 6(h), and 6(i), the red
and black arrows are marked to indicate that the resistivity was
measured by warming and cooling under zero magnetic field, respec­
tively. Regardless of the directions of the magnetic field, the thermal
hysteresis effects are observed for all films, which strongly indicates that
the FIM(II)-to-c-AFM magnetic phase transition near 150 K is of first
T.-W. Chen et al. Acta Materialia 259 (2023) 119257

Fig. 6. Temperature dependence of the field-cooling and field-warming resistivity of Mn2Sb films with various thicknesses. (a-e) Out-of-plane ρ-T curves of the 8, 12,
16, 32, and 64-nm Mn2Sb films, respectively. (f-j) In-plane ρ-T curves of these Mn2Sb films.

6
T.-W. Chen et al.
order, which has yet not been reported in Mn2Sb bulk.
To further study the reasons for the discrepancy in the electronic and
magnetic properties between the Mn2Sb films and Mn2Sb bulk, we
prepared Mn2Sb films with difference thicknesses t (8 ≤ t ≤ 64) on STO
(001) substrates using the same growth recipe. The XRD θ− 2θ patterns
of these thin films are shown in Fig. S5 (Supporting Information), which
indicates that all films are single phase and c-axis oriented. The XRD
rocking curve, XRR, and AFM images of them are shown in Fig. 7.
FWHMs of the rocking curves taken on the Mn2Sb (002) diffraction peak
are 1.07◦ , 0.13◦ , 0.10◦ , 0.19◦ and 0.24◦ for the 8, 12, 16, 32, and 64 nm
Mn2Sb films, respectively, which demonstrates that they have good
crystallization quality. The XRR patterns indicate that the films with
different deposition times have different thicknesses, ranging from ~8
to 64 nm. The atomic force microscopy images show that the roughness
of the 8, 12, 16, 32, and 64-nm Mn2Sb films are 0.97, 1.01, 0.30, 1.37,
and 1.45 nm, respectively. We note that the 2θ angles of the XRD (00l)
peaks of the thickest Mn2Sb film (64 nm) are close to those of the bulk.
For thinner films (< 64 nm), the XRD θ− 2θ scan peak positions increase
with decreasing film thickness, indicating a decrease in the lattice con­
stant c. The lattice constant c of the 8-nm Mn2Sb film at 300 K is 6.427 Å,
smaller than 6.56 Å of the Mn2Sb bulk [Fig. 8(a)]. Interestingly, we
found that the anomalous Hall resistivity (ρAH ) at 300 K is related to the
thickness of the films [Fig. 8(a)], namely, AHE in thinner film is quite
significant, and decreases with increasing film thickness. Temperature
dependence of ρAH of Mn2Sb films with various thicknesses is shown in
Fig. 8(b). Here, ρAH is extracted from the anomalous Hall effect curves
shown in Figure S6 (Supporting Information). ρAH of the 8-nm film in­
creases near-linearly with the temperature and are significantly larger
than those of the other thin-film samples, and shows a maximum value
of 1.48 μΩ cm at 300 K. While ρAH of the 64-nm film has a maximum
value of 0.67 μΩ cm at 175 K, which is the spin reorientation transition
temperature of the Mn2Sb film. Upon cooling, ρAH of the 64-nm film
decreases to almost 0 μΩ cm at 2 K [Fig. 8(b)], where the Mn2Sb film
enters into the c-AFM state. According to the out-of-plane magnetic
hysteresis loops of Mn2Sb films at various temperatures (Figure S7,
Supporting Information), the out-of-plane saturation magnetization for
various film thicknesses are extracted and plotted against temperature in
Fig. 8(c). One may notice that, the 8-nm film has an abnormally large
saturation magnetization (4.8 μB/f.u.), which is 5.5 times larger than
that of Mn2Sb bulk (~1.74 μB/f.u.) [32]. For the 16-nm Mn2Sb film, the
saturation magnetization Msat increases with cooling in the high tem­
perature FIM region (300 - 170 K), and shows a maximum value of 2.70
μB/f.u. at 170 K, and slightly increases to 2.71 μB/f.u. at 140 K. Upon
further cooling, Msat decreases to 1.86 μB/f.u. at 10 K due to the tran­
sition to the c-AFM phase. With increasing film thickness from 8 to 64
nm, Msat decreases proportionally (especially at low temperatures, e.g.,
10, 20 K) and evolves toward 0.5 μB/f.u. at 10 K for the 64-nm film
[Fig. 8(c)]. Therefore, with decreasing film thickness, both Msat and ρAH
increases in general. It is inferred that the abnormally large ρAH for the
8-nm films should be derived from its giant Msat. In contrast, with
decreasing film thickness, the resistivity changes (ΔR) associated with
the FIM(II)-to-c-AFM phase transition near 150 K decrease (Figure S8,
Supporting Information), indicating a suppression of the phase transi­
tion, which may be due to the enhancement of interfacial strain effect
with decreasing film thickness.
The enhanced anomalous Hall effect and remanent magnetization
with decreasing film thickness is probably related to the interfacial
epitaxial strain which would modify the spin aligned at the interface
region. Note that the epitaxial strain relaxes quickly in the thickness of
approximately a few nanometres due to the large lattice mismatch
(~5.7%) between the STO and Mn2Sb. The is evidenced by the increased
FWHM of rocking curve for the 8-nm film [Fig. 7(a)] and a quick
decrease in the lattice constant c with increasing film thickness [Fig. 8
(a)]. We have carried out the first-principles calculations based on the
DFT to demonstrate the effects of interfacial strain on the spin canting in
thinner films. We simulate the interface between Mn2Sb and STO (left
7
Acta Materialia 259 (2023) 119257
panel of Fig. 9). The lattice mismatch between STO and Mn2Sb (001) at
the ground state (0 K) is only 0.28%, indicating that the two lattices can
be perfectly matched. To avoid interlayer coupling induced by the
period boundary condition, we set at least 20 Å vacuum layer at the Z
direction perpendicular to the XY contact interface. During the struc­
tural optimization, STO substrate and the top three layers of Mn2Sb
atoms are fixed, leaving the interfacial three-layer Mn2Sb (one period)
free to relax. The results show that the Sb and Mn atoms at the interface
have obvious position shift (right panel of Fig. 9). As a result, the
magnetic moments of the Mn atoms are no longer stay in the ab plane.
The direction of moments has a certain inclination angle with respect to
the ab plane (more than 0.5 μB along the Z direction), which is consistent
with the abnormally large magnetization in the 8-nm film. As the film
thickness increases, the magnetization due to the spin canting at the
interface region will be diluted, resulting in the decreased magnetization
with increasing film thickness [Fig. 8(c)].
The thickness dependent lattice constant, ρAH , and magnetization
[Fig. 8(a), 8(b), 8(c)] suggest that the shrinkage of the lattice constant c
significantly enhances the anomalous Hall effect and ferromagnetism,
implying strong spin-lattice coupling effects. Such effects are also
manifested by the variation of the in-plane and out-of-plane ZFC
magnetization with temperature, as shown in Fig. 10(a) and 10(b),
where both the in-plane and out-of-plane remanent magnetization in­
creases considerably with decreasing film thickness. Since all films with
different thicknesses are single phase, the influences of impurity phases
on the magnetic properties can be excluded. It is believed that the
thickness dependent remanent magnetization is due to the interfacial
lattice strain. As the film thickness decreases, the contribution of the
magnetization from the strain layer near the interface becomes more
significant to the total magnetization, leading to an increase in the
remanent magnetization. Furthermore, the magnetization change near
the magnetic phase transitions is more pronounced for thicker films, e.
g., the 24-nm film in Fig. 10(a). We therefore plot the magnetization and
magnetic phases of the 24-nm Mn2Sb film in the temperature range from
360 to 2 K in Fig. 11(a), where two magnetic transitions and three
phases can be identified as (1) the ferrimagnetic phase FIM(I) phase with
out-of-plane spin orientation (approximately > 260 K); (2) SR region
(approximately 150–260 K) where the direction of spins rotates from
out-of-plane to in-plane, as reflected by the rapid decrease in the out-of-
plane magnetization below 260 K and increase in the in-plane magne­
tization, resulting in the FIM(II) phase with in-plane spin orientation; (3)
FIM(II)-to-c-AFM phase transition region (115–150 K) where the in-
plane magnetization decreases rapidly, signaling the formation of c-
AFM phase; (4) the c-AFM phase region (<115 K) where the out-of-plane
moment approaches zero at 10 K while the in-plane net moment is 0.39
μB/f.u. at 10 K. The net moment is probably contributed by canted spin
moments within the ab plane of the Mn2Sb film, which is allowed when
an in-plane DM interaction occurs by interface mismatch at low tem­
peratures. [66,67]
The temperature dependent out-of-plane lattice constant c are shown
in Fig. 11(b), to demonstrate the lattice behaviours of different phases.
We focus on the anomalous FIM(II)-to-c-AFM phase transition. Previous
work reported that this phase transition is only observed in transition-
metal-doped Mn2Sb bulk materials [68,69] and is accompanied with
the contraction of the lattice constant c. We measured the lattice con­
stant c of the Mn2Sb film via XRD in the 50–300 K region, and show the
XRD patterns in the heat map format in the inset of Fig. 11(b). At T =
300 K, the lattice constants a and c are calculated to be 4.12 Å and 6.51 Å
by combining the out-of-plane and in-plane XRD pattern (Figure S9,
Supporting Information), respectively, indicating an in-plane expansion
by 1% and out-of-plane contraction by 0.8%, respectively. Upon cooling
from 300 to 130 K, the lattice constant c decreases almost linearly with a
coefficient of thermal expansion ~1.7 × 10− 5/ ◦ C, which is slightly
larger than that (1.4 × 10− 5/ ◦ C) of Mn2Sb bulk. [70] In addition, we
have grown Mn2Sb films on (001)-oriented GdScO3 (ap=3.96 Å) sub­
strates with larger lattice constants. The FIM(II)-to-c-AFM phase
T.-W. Chen et al. Acta Materialia 259 (2023) 119257

Fig. 7. XRD rocking curve, XRR, and AFM images of Mn2Sb films with various thicknesses. (a-e) Rocking curve of the 8, 12, 16, 32, and 64-nm Mn2Sb films,
respectively. (f-j) XRR patterns of these Mn2Sb films. (k-o) The AFM images of these Mn2Sb films.

8
T.-W. Chen et al. Acta Materialia 259 (2023) 119257

Fig. 9. The DFT calculation model for Mn2Sb/STO structure. Left panel:
structure before optimization. Right panel: structure after optimization.

Fig. 8. (a) Thickness dependence of lattice constant c and anomalous Hall re­
sistivity at room temperature for Mn2Sb films. (b) Temperature dependence of
anomalous Hall resistivity for various film thicknesses. (c) Temperature
dependence of the out-of-plane saturation magnetization for various film
thicknesses.

transition of Mn2Sb films on these substrates can still be observed at

similar temperature region (Figure S10, Supporting Information). Fig. 10. Temperature dependence of zero-field-cooled magnetization for
Since the thermal expansion coefficient of STO oxide is much smaller Mn2Sb films with various film thickness. The magnetic field of 500 Oe is applied
than that of Mn2Sb alloy, the already expanded in-plane lattice of the along (a) the in-plane direction and (b) the out-of-plane direction.
Mn2Sb films at the growth temperature (330 ◦ C) will be partially
clamped by the STO substrates. This clamping effect will prevent the
film’s ab plane from shrinkage freely as the temperature decreases from

9
T.-W. Chen et al.
Fig. 11. (a) Schematic diagram of the magnetic phases, together with the out-
of-plane and in-plane magnetization in the temperature region below 360 K, as
measured in the zero-field-cooled mode with B = 500 Oe. (b) The ut-of-plane
lattice constant c plotted against temperature. Inset: XRD 2D contour plot.
the growth temperature to room temperature, meanwhile the out-of-
plane lattice constant c would shrink more significantly to maintain its
lattice volume, as schematically shown in Fig. 12. Upon further cooling
from room temperature to lower temperatures, the lattice constant c
continues to shrink and show rapid shrinkage below 130 K where FIM
(II)-to-c-AFM phase transition occurs. Note that our computational re­
sults show that, compared to the antiferromagnetic order, the ferro­
magnetic energy of free-Mn2Sb in the ground state is slightly lower,
indicating that the magnetic moment arrangement is ferrimagnetic
without clamping effect. However, taking into account the substrate
clamping effect, we apply a strain on the a and b axis of Mn2Sb to stretch
the lattice by 1%, and then optimize the structure. The optimized
structure does have a clearly decreased lattice constant of the c-axis
(Fig. 13), and the ground state becomes antiferromagnetic order because
Fig. 12. Schematic of the substrate clamping effect. (a) The lattice constant a,
b, and c of Mn2Sb films expand at the growth temperature of 330 ◦ C due to the
thermal expansion effect. (b) Upon cooling from the growth temperature to
room temperature, the in-plane lattice is clamped by the STO substrate. This
will prevent the film’s ab plane from shrinkage freely, meanwhile the out-of-
plane lattice constant c would shrink more significantly in order to maintain
its lattice volume.
10
Acta Materialia 259 (2023) 119257
Fig. 13. The DFT calculation model for strain free Mn2Sb lattice (left panel).
The model for ab plane expansion and c-axis contraction (right one). The lattice
constants are the optimized results. The calculation results show that the
ground state of stain free one is FIM, and of strained one is AFM.
the contraction of the lattice constant c will enhance the indirect ex­
change interaction via Sb 5p states -between neighbouring magnetic
sublattices, and thus converts the coupling from FIM to AFM of adjacent
magnetic sublattices [30,46,68,69]. Since the growth temperature for all
films is the same (330 ◦ C), the lattice expansion during thin-film growth
process would be similar, and moreover, the clamping effect can be
maintained over hundreds of nanometers thickness [71,72]. Therefore,
the clamping effects of the 8–64 nm Mn2Sb films are similar, which may
lead to similar FIM(II)-to-c-AFM phase transition temperatures for
Mn2Sb films with different thicknesses and even on different substrates.
4. Conclusions
In summary, high quality Mn2Sb epitaxial films are grown on
perovskite STO (001) single-crystal substrates via precise control of the
growth parameters using molecular beam epitaxy. Magnetotransport,
anomalous Hall effect, and magnetic measurements demonstrate that
upon cooling, a spin reorientation transition from the FIM(I) phase with
out-of-plane spin configuration to the FIM(II) phase with in-plane spin
configuration occurs approximately in the 150–260 K temperature re­
gion. Below 150 K, a giant magnetoresistance accompanied anomalous
FIM(II)-to-c-AFM phase transition occurs, resulting in the c-AFM ground
state, which is completely absent and has not yet been observed in
Mn2Sb bulk and thin films grown on other substrates. The stabilization
of the low temperature c-AFM phase is attributed to the enhanced in­
direct exchange interaction via Sb 5p states between neighbouring
magnetic sublattices, arising from the shrinkage of the lattice constant c
by substrate clamping, below the phase transition temperature. In the c-
AFM ground state, the 24-nm Mn2Sb film shows almost zero out-of-plane
moment and appreciable remanent in-plane moment and anomalous
Hall effect, implying spin canting within the ab plane of the film. Both
the anomalous Hall resistivity and saturation magnetization increases
with decreasing film thickness from 64 to 8 nm. The low temperature
saturation magnetization of the 8-nm film is 2.8 times larger than that of
Mn2Sb bulk and 10 times larger than that of the 64-nm one, both of
which are attributed to the interfacial strain effect. Our systematic work
on the growth and electronic and magnetic properties of Mn2Sb films
provides useful reference for growing high quality Mn2Sb-based films on
perovskite oxide substrates and the exploration of its potential device
applications.
CRediT authorship contribution statement
R.K.Z. and W.Z. supervised the research. T.W.C. prepared thin films
T.-W. Chen et al.
and measured electronic properties. S.L. conducted DFT calculations. F.
T. and Y.F. performed magnetic measurements, Y.Z., S.S.L, L.C., and J.S.
Y. did XRD, AFM, and EDS measurements. S.K. contributed to discus­
sion. T.W.C., W.Z. and R.K.Z. wrote the manuscript with input all au­
thors. All authors discussed the results and commented on the
manuscript.
Declaration of Competing Interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
the work reported in this paper.
Acknowledgments
This work is supported by National Natural Science Foundation of
China (Grant No. 11974155) and the Creative Project for Graduate
Students of Jiangxi Province (No. YC2020-B010), and Bureau of Edu­
cation of Guangzhou Municipality (Grant No. 202255464). We grate­
fully acknowledge HZWTECH for providing computation facilities.
Supplementary materials
Supplementary material associated with this article can be found, in
the online version, at doi:10.1016/j.actamat.2023.119257.
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