RESEARCH ARTICLE | AUGUST 13 2018
Electrical and anisotropic magnetic properties in layered
Mn1/3TaS2 crystals
Hongwei Zhang ; Wensen Wei ; Guolin Zheng; Jianwei Lu; Min Wu; Xiangde Zhu; Jin Tang ;
Wei Ning ; Yuyan Han; Langsheng Ling; Jiyong Yang; Wenshuai Gao; Yongliang Qin; Mingliang Tian
Appl. Phys. Lett. 113, 072402 (2018)
https://doi.org/10.1063/1.5034502
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02 April 2025 06:47:14
APPLIED PHYSICS LETTERS 113, 072402 (2018)
Electrical and anisotropic magnetic properties in layered Mn1/3TaS2 crystals
Hongwei Zhang,1,2 Wensen Wei,1 Guolin Zheng,1 Jianwei Lu,1,2 Min Wu,1,2 Xiangde Zhu,1
Jin Tang,1 Wei Ning,1 Yuyan Han,1 Langsheng Ling,1 Jiyong Yang,1 Wenshuai Gao,1,2
Yongliang Qin,1 and Mingliang Tian1,3,a)
1
The Anhui Province Key Laboratory of Condensed Matter Physics at Extreme Conditions, and High Magnetic
Field Laboratory, Chinese Academy of Sciences (CAS), Hefei 230031, Anhui, China
2
Department of Physics, University of Science and Technology of China, Chinese Academy of Sciences (CAS),
Hefei 230026, Anhui, China
3
School of Physics and Materials Science, Anhui University, Hefei 230601, China
(Received 12 April 2018; accepted 19 July 2018; published online 13 August 2018)
We report electrical transport and anisotropic magnetic properties of Mn-intercalated 2H-TaS2, a
layered transition-metal dichalcogenide with a hexagonal structure. The single crystal MnxTaS2
with x ¼ 1/3 exhibits a transition from paramagnetism to ferromagnetism near 70 K, below which
both the magnetoresistance and magnetization properties present strong anisotropic behavior. Its aniso-
tropic magnetoresistance effect and in-plane soft ferromagnetic property suggests that this layered
material would be a good candidate for exploring the physics of two-dimensional ferromagnetism.
Published by AIP Publishing. https://doi.org/10.1063/1.5034502
The transition metal dichalcogenides (TMDs) have studied for many decades, the magnetotransport and mag-
attracted considerable attention over the past three decades netic properties of Mn1/3TaS2 still remain elusive.13,14,16,24,25
due to their simple crystal structures and rich physical prop- In this work, we systematically investigated the magneto-
erties. They cover wide kinds of physical properties includ- transport properties of 2D van der Waals ferromagnetic crys-
ing insulators (HfS2), semiconductors [MX2 (M ¼ Pt, Pd, tal Mn1/3TaS2 and found unusual magnetoresistance (MR)
Mo and X ¼ S, Se)], semimetals (WTe2, TcS2), metals and anisotropic magnetic properties.
(NbS2, VSe2), and superconductors (TaS2, TaSe2, NbSe2).1–6 The single crystal of Mn1/3TaS2 was grown by chemical
02 April 2025 06:47:14
These materials exhibit not only interesting physics but also vapor transport method with iodine agent. First of all, a stoi-
potential applications. One of the most interesting features is chiometric mixture of Mn, Ta, and S with a mole ratio of
that the intercalation of different kinds of atoms between 1:3:6 was ground into powder, followed by mixing an appro-
MX2 layers leads to significant changes in their physical priate amount of iodine. Second, the powder was put into an
properties, such as superconductivity,7–11 and semiconductor- evacuated quartz tube and was heated for 10 days in a two-
metal transition. More interestingly, a long-range magnetic zone furnace with the source zone temperature of 1260 K
order can be realized by intercalating 3d-transition metal and the growth zone temperature of 1170 K. The obtained
atoms such as Mn, Fe, Co, and Ni12–14 among the MX2 Mn1/3TaS2 plates were cleaned by ultrasonication in super-
layers. The structural and magnetic properties of the interca- saturated aqueous solutions of KI, de-ionized water, and
lated TxMX2 (T: 3d-transtion metals) depend strongly on the alcohol. The obtained single crystals show a thick, hexagonal
amount of the intercalant concentration x.15–17 For instance, shape with length up to several millimeters. The structures of
when x ¼ 1/4, TxMX2 turns out to be a compound pffiffiffi pwith
ffiffiffi Mn1/3TaS2 single crystals were characterized by X-ray
2a0 2a0 superstructure, while for x ¼ 1/3, a 3a0 3a0 diffraction (XRD) at room temperature. The magnetization
superstructure is formed, where a0 is the lattice parameter of measurements were performed on the Superconducting
hexagonal basal plane of MX2.18,19 T1/3MX2 is reported to Quantum Interference Device (SQUID) system. Temperature-
show some distinct magnetic properties, such as Cr1/3NbS2 dependent resistivity measurement was performed by using a
shows left-handed spin helices. Other compounds of similar standard four-point probe technique in the Physical Property
structures such as Cr1/3TaS2, V1/3TaS2, V1/3NbS2, Ti1/3NbS2, Measurement System (PPMS) with a magnetic field up to 7 T.
20
Cr1/3NbSe2, and Cr ffiffiffi TaSe
p1/3 p2ffiffiffi are also reported. In addition, Figure 1(a) shows the XRD pattern at room tempera-
Co1/3TaS2 has a 3 3 magnetic supercell that corre- ture for Mn1/3TaS2 single crystals, all the peaks can be
sponds to a triangular antiferromagnetic structure, which is a indexed with (00l) planes, which is consistent with the
particularly uncommon structure.21 previous work.26 Fitting the XRD data, the lattice parame-
27
Mn1/3TaS2 is a two-dimensional (2D) van der Waals ters, a ¼ 5.833 Å and c ¼p12.559
ffiffiffi pÅ,
ffiffiffi were obtained. The
material with a ferromagnetic ground state. Recent realiza- parameter a is close to 3a0 3a0 superstructures pat-
tion of ferromagnetism (FM) in monolayer van der Waals tern, where a0 is the lattice parameter of hexagonal basal
crystal CrI322 and bilayer Cr2Ge2Te623 has further triggered plane of MX2, which is consistent with the previous litera-
the enthusiasm in 2D van der Waals ferromagnetic materials. tures.13,14,16,24,25 The inset of Fig. 1(a) shows a photo-
Although the transition metal dichalcogenides have been graph of Mn1/3TaS2 single crystal, and it shows navy blue
color with a hexagonal shape. Figure 1(b) presents the
a)
Author to whom correspondence should be addressed: tianml@hmfl.ac.cn temperature-dependence of in-plane resistance (R), where
0003-6951/2018/113(7)/072402/4/$30.00 113, 072402-1 Published by AIP Publishing.
072402-2 Zhang et al. Appl. Phys. Lett. 113, 072402 (2018)
kink around T ¼ 35 K. Figures 2(c) and 2(d) show the field
dependent magnetization (M-H) at different temperatures
with the magnetic field perpendicular and parallel to the
ab-plane, respectively. When the magnetic field is along the
c-axis, the magnetization Mc slowly reaches the saturation
at about 6 T at 2 K. While applying the magnetic field in
ab-plane, the magnetization Mab increases sharply and satu-
rates around 0.6 T. No obvious hysteresis loop was recognized
near H ¼ 0 Oe, but a tiny loop occurs near the saturation field
Hs at 2.0 K as shown in the inset of Fig. 2(d). This result is
FIG. 1. (a) X-ray diffraction pattern of Mn1/3TaS2 single crystal at 300 K.
The left inset is a photo of the grown Mn1/3TaS2 single crystals. (b)
similar to previous measurements in Cr1/3NbS2.28,29
Temperature-dependence of in-plane resistance (R), and the right inset In order to give more information on the anisotropic
shows the curve of dR/dT versus temperatures. magnetization in this Mn-doped ferromagnetic system, we
measured the angle-dependent magnetization as a function
an anomaly of R near 70 K was observed, which can be of angle h in ac-plane and u in ab-plane at 2 K under mag-
clearly defined as shown in the inset of Fig. 1(b). netic fields, 0.05 T and 1.0 T, as shown in Figs. 2(e) and 2(f).
Figures 2(a) and 2(b) depict the temperature- Here, h is defined as the angle between H and ab-plane, and
dependence of the magnetization measured at an applied u is the rotation angle of H in the ab-plane. It was seen that
magnetic field of 100 Oe oriented parallel to the c-axis (Mc) the magnetization in the ac-plane exhibits a twofold symme-
and along the ab-plane (Mab) with both zero-field cooling try, suggesting a very strong magnetic anisotropy. However,
(ZFC) and field cooling (FC), respectively. A sharp upturn of when the magnetic field rotates in ab-plane, the magnetiza-
Mab and Mc was observed below Tc 70 K, followed by a tion shows an isotropic behavior. For the saturation field Hs
02 April 2025 06:47:14
FIG. 2. (a) and (b) show the
temperature-dependent magnetization
with zero-field (black line) and field
cooling process (red line) for both the
H//c-axis and H//ab-plane, respectively;
(c) and (d) are the corresponding aniso-
tropic field-dependent magnetization at
different temperatures, respectively. The
inset in (d) is the enlarged M-H curve
near the saturation field at 2 K. (e) and
(f) are the angular dependent magnetiza-
tion in ac and ab-planes at 2 K measured
under magnetic fields,0.05 T and 1 T for
Mn1/3TaS2, respectively.
072402-3 Zhang et al. Appl. Phys. Lett. 113, 072402 (2018)
in the ab-plane is much smaller than that along the c axis, we 3(c) shows the experimental data gained from Fig. 3(a) and
can easily draw a clear conclusion that Mn1/3TaS2 single the fit with Eq. (1). In the fitting, we define s ¼ 1/f and Tf
crystal is ferromagnetic below about 70 K with its magnetic ¼ Tmax. The fitting gets s0 ¼ 1:3 109 s, Tg ¼ 48:9 K, and
moments tending to be arranged in the ab-plane and the zv ¼ 4.05. Both s0 and zv values are falling into the charac-
c-axis is the magnetic hard axis, but the magnetically easy teristic range of cluster spin glass state, confirming that
axis in the ab-plane is not along a specific axis. cluster spin glass state emerges in Mn1/3TaS2. We attribute
Note from Figs. 2(a) and 2(b) that there is a bifurcation this cluster spin glass to the inhomogeneity of the Mn-
between ZFC and FC curves. This behavior is reminiscent of intercalation, and the strong FM anisotropy in magnetization
spin glass state, but also quite puzzling by the observation of is the consequence of the quasi-2D nature of the Mn-
the strong magnetization anisotropy. To clarify this, ac mag- intercalation between the TaS2 layers.
netic properties with H//ab-plane and H//c were measured Figures 4(a) and 4(b) present the MR properties under
with various ac driving frequencies, as shown in Figs. 3(a) various temperatures with current injected in ab-plane, and
and 3(b). We can see that no matter for H//ab-plane or H//c, the magnetic field applied parallel to the ab-plane and c-axis,
a peak below Tc is observed at all frequencies and the posi- respectively. The MR with the H//ab-plane shows a negative
tion of the peaks shifts to low temperatures with the decrease behavior over the entire temperatures, and a sharp cusp near
in the driving frequency. This frequency-dependent phenom- H ¼ 0 Oe was observed at low temperatures. This negative
enon intuitively indicates a spin glass-like character. Note MR property is well expected in an in-plane polarized FM
that the typical spin glass state should not have such strong thin film system.33,34
anisotropy in magnetization; observation of the strong In contrast, when H//c-axis, a positive MR with a
anisotropy in magnetization suggests possible existence of plateau or a broad shoulder was observed below 70 K in low-
cluster spin glass in the in-plane ferromagnetic states in field region, as depicted in Fig. 4(b). This positive MR then
Mn1/3TaS2. decreases significantly with a further increase in the mag-
To verify the conclusion mentioned earlier, we fit our netic fields and it nearly saturates at H > Hs. Both the values
frequency dependent experimental data with the power law of Hc and Hs increase with the decrease in temperatures. The
model.30 This model bases on scaling hypothesis and states value of Hs is consistent with that measured from the M-H
that the characteristic relaxation time near the transition tem- data in Fig. 2(c). The plateau or slight positive MR below Hc
perature is linked to the spin cluster correlation length n suggests the enhancement of the scattering which is hardly
02 April 2025 06:47:14
according to s / nz.31,32 Because n is divergent at the transi-
interpreted by the partially polarization of magnetization
tion temperature, the temperature dependence of the relaxa-
along the c-axis. Interestingly, the feature of MR with the
tion time s, close to critical temperature region, is expected
H//c-axis is very similar to that observed in helical magnetic
to follow
MnSi nanowire, where magnetic field-induced conical or
zv skyrmion phase occurs.35 The plateau behavior of the MR
Tf
s ¼ s0 1 ; (1) below 70 K might be related to some field-induced novel
Tg
magnetic structures, which have not been recognized at
where Tg is the freezing temperature, s0 is related to the present. When temperature reaches above 150 K, the para-
relaxation of individual cluster magnetic moment, and zv is a magnetic order is dominant, and the MR effect is almost
critical exponent and its value ranging from 4 to 12.30 Figure field-independent.
FIG. 3. (a) and (b) are the ac susceptibility on Mn1/3TaS2 with ac magnetic
field along the ab-plane and c-axis, respectively. The amplitude of ac field is
1 Oe and all the measurements are taken without any dc magnetic field. The
insets in (a) and (b) are the enlarged part of the related peak region, respec- FIG. 4. (a) and (b) are the field-dependence of magnetoresistance with
tively. (c) is the relaxation time, s ¼ 1/f, versus temperature, Tmax, obtained current injected in the ab-plane for the H//ab-plane and H//c-axis at various
from (a). temperatures, respectively.
072402-4 Zhang et al. Appl. Phys. Lett. 113, 072402 (2018)
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