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Low-field anomalous magnetic phase in the kagom-lattice shandite Co3Sn2S2

Mohamed A. Kassem*,, Yoshikazu Tabata, Takeshi Waki, Hiroyuki Nakamura


Department of Materials Science and Engineering, Kyoto University, Kyoto 606-8501, Japan.
Abstract
The magnetization process of single crystals of the metallic kagom ferromagnet Co3Sn2S2
was carefully measured via magnetization and AC susceptibility. Field-dependent anomalous
transitions in the magnetization indicate a low-field unconventionally ordered phase stabilized
just below TC. The magnetic phase diagrams in applied fields along different crystallographic
directions were determined. The magnetic relaxation process studied in frequencies covering
five orders of magnitude from 0.01 to 1000 Hz indicates characteristic relaxation times of
several seconds at the boarders of the anomalous phase. Our results arise a lot of questions
about the nature of Co3Sn2S2 magnetic states.
1. Introduction
The kagome-lattice, a 2-dimensinal (2D) studies of the magnetization process of the
conner-sharing triangular-lattice, is a platform of halfmetallic ferromagnet Co3Sn2S224,25 have explored
many exotic phenomena originated from its geometry. high axial anisotropy in magnetization M(T, H)26,27.
For instance, antiferromagnetic-coupled spin system The Curie temperature, TC, and the spontaneous
on the kagom-lattice is highly-frustrated and can moment at 2 K in the easy c-axis were reported as 174
exhibit quantum disordered spin liquid1 and exotic K and ~ 0.3 B/Co, respectively. Recent
magnetic ordered states with non-trivial spin comprehensive magnetization measurement and
textures25. The geometric spin frustration is one of analysis based on the spin fluctuation theory revealed
the most intriguing issues in recent condensed matter the quasi-two-dimensionality (Q2D) of the
physics69. The asymmetric Dzaloshinski-Moriya magnetism in Co3Sn2S2 and its In-substituted
(DM) interaction is another driving force of non- system28. This implies that Co3Sn2S2 is a model
trivial spin textures in the kagom-lattice magnets811. system of the 2D kagom-lattice ferromagnet and has
The DM interaction can destabilize collinear ferro- a potential to exhibit exotic magnetic states with
and antiferromagnetic orders and results in spiral and nontrivial spin textures.
canted spin structures. Furthermore, a topologically-
protected vortex-like spin texture, called as
"skyrmion", is also induced by the DM interaction.
Theoretically, spontaneous triangular-lattice
formation of skyrimons was proposed in the presence
of the DM interaction based on the phenomenological
continuum model12. Indeed, the skyrmion-lattice
phase was experimentally observed in
1317 18
noncentrosymmetric chiral and polar crystals
under finite field and in the vicinity of TC.
Co3Sn2S2 consists of Co-Sn metallic layers,
stacked along c-axis in the hexagonal setting of R3m
structure, that are separated by Sn-S blocks1924. In Figure 1: Crystal structure projection in (001)-plane
each layer, Co atoms are arranged in a 2D-kagom showing a Co-kagom sublattice in Co3Sn2S2.
sublattice as shown in Fig. 1. Previously reported

1
In this paper, we present results of applied along and perpendicular to the c-axis are
magnetization, M(T, H), and AC susceptibility, ac(T, shown in Figs. 2(a) and (b). Both axial and in-plane
H), of Co3Sn2S2 systematically accumulated at low- magnetizations, Mc and Mab, show sharp increases at
fields and clearly indicate low-field anomalous TC ~ 173 K, which correspond to the previously
magnetic phase just below TC. The anomalous phase reported ferromagnetic phase transitions24,26,27,29. As
shows slow dynamics indicating a frozen magnetic in literature, strong magnetic anisotropy below TC
state with characteristic relaxation times longer than was confirmed below TC. The difference is reduced
10 sec. with increasing of magnetic field and disappears
above ~1k Oe in the axial magnetization.
2. Experimental Details
Interestingly, peculiar anomalies were found
Single crystals of Co3Sn2S2 used in this work at low field where the ZFC and FC magnetizations
have been grown by a flux method29,30. separate from each other. The axial magnetization, Mc
Magnetization processes were measured using a (T, H) in the FC process shows a hump-anomaly at
SQUID magnetometer (MPMS, Quantum Design) temperature TA ~ 126 K with applying H = 5 Oe,
with magnetic fields applied parallel and indicating another magnetic transition apart from the
perpendicular to the easy c-axis. For the AC transition at TC. The anomaly-temperature, TA,
susceptibility measurements, 1 Oe drive AC field of slightly increases with the increasing of H. On the
different frequencies was superimposed on the bias other hand, the ZFC magnetization shows a dip-like
field and both were applied along the c-direction. anomaly in the intermediate temperature range
Two experimental regimes have been followed in the between TA and TC. Both the hump-anomalies in FC
measurement of temperature-scans: (i) Zero-field-
cooled (ZFC) scans, after resetting the magnetometer
to zero field, the sample was brought to 5 K under
zero field. The magnetic fields were applied at 5 K
and the measurement were performed by increasing
stepwise the temperature, after thermal equilibrium
was reached at each temperature. (ii) Field-cooled
(FC) scans, in which the sample was cooled from 250
K, where the DC and/or AC magnetic fields were
applied, and the measurement was performed with
decreasing stepwise the temperature. At each
temperature the sample was brought to thermal
equilibrium before the measurement.
The spin relaxation processes at selected
temperatures were systematically studied by
measuring the ZFC AC susceptibility for different
magnetic fields in a frequency range of five orders of
magnitude from 0.01 to 1000 Hz. For the frequency
scans, the above ZFC regime was followed and the
fields were applied at the temperature of interest
before the measurement. Figure 2: The temperature dependences of ZFC and FC
magnetizations, M(T, H), of Co3Sn2S2 measured at the
3. Results indicated low magnetic fields applied (a) along and (b)
3.1. Magnetization perpendicular to the c-axis. The vertical arrows indicate
The temperature dependences of the ZFC and the transition temperature TA and the broad minimum
FC magnetizations M(T, H) of Co3Sn2S2 single (see text). The inset of (b) shows a magnification of the
crystal measured at various low magnetic fields ZFC M(T) measured at very low fields.

2
Mc (T, H) and the minimum in the ZFC Mc (T, H) Figure 4 shows the temperature dependences
disappear at H 400 Oe. One can note that the of the ZFC and FC real and imaginary parts of the AC
anomalies are observed at fields below the saturation susceptibility, c'(T, H) and c"(T, H), with f = 1, 10,
fields of Co3Sn2S228. 100 and 1000 Hz under several DC fields applied
The in-plane magnetization, Mab(T, H), along the c-axis. The characteristic features in c' with
displayed in Fig. 2(b), shows similar hump-anomaly f = 1 Hz at 150 Oe, found in Fig. 3, are recognized for
at TA in the FC process and dip-like anomaly between all frequencies at low field (0 and 150 Oe), as shown
TA and TC. in the ZFC process. Additionally, the ZFC in Figs. 4 (a) and (c). At 600 Oe, shown in Fig. 4 (e),
Mab(T, H), also shows a hump-like anomaly at TA at only the anomaly at TC is found. Absence of the
very low fields (below 150 Oe), as seen in the inset hump-like anomaly and broad minimum is also
of Fig. 2(b). The field-dependences of the peculiar recognized in the dc magnetization at higher than 400
anomalies in Mab are more gentle than those in Mc. Oe. The anomaly at TC at 600 Oe is rather broaden,
Especially, the dip-like anomaly in the ZFC process which suggests a difference of the natures at low and
is still observable above 400 Oe. high fields. It should be noted c' in the ZFC and FC
processes almost coinside each other at low and high
3.2. AC susceptibility of Co3Sn2S2
fields, unlike the dc magnetization.
For more detailed investigation of the The characteristics at low field are more
magnetic transitions observed just below TC, we have pronounced in the imaginary part of the ac
carefully measured the temperature-, field- and susceptibility, c", as shown in Figs. 4 (b) and (d). c"
frequency-dependences of the AC susceptibility, ac, is almost absent above TC and shows more rapid
after ZFC and FC in a wide range of frequencies f increasing at TC than c'. The anomalies below TC in
from 0.01 to 1000 Hz. Figure 3 shows the temperature c" are not so distinct as in c', except for that with 1Hz.
dependence of the ZFC in-phase AC susceptibility, More than that, it should be emphasized that c" is
c'(T), measured with a frequency of 1 Hz and H =150 considerably recognized only between TA and TC. At
Oe applied along the c-axis. For comparison, the ZFC 600 Oe, c", is almost absent regardless of temperature
magnetization Mc(T) measured at the same conditions
and frequency, At 600 Oe, c" is almost absent
is shown. c' shows distinct anomalies as well as regardless of temperature and frequency, as shown in
observed in the dc magnetization: a sharp peak at TC, Fig. 4 (f). The existence of c" with the frequcency
hump-like anomaly at TA and a broad minimum
region of 1 1000 Hz indicates that spin dynamics
between TA and TC.
slows down to the time scale of 0.001 1 s only
between TA and TC in low field. It is a clear evidence
of emergence of the anomalous phase apart from a
conventional ferromagnetic ordered state in Co3Sn2S2.
3.3. Magnetic phase diagrams
Here we present the magnetic phase diagrams
of Co3Sn2S2 based on the magnetization and AC
susceptibility data descripted above. Figure 5(a)
illustrate the H-T phase diagram in the case of applied
magnetic fields along the c-axis. In the phase
diagram, TC and TA obtained from the FC
magnetization and ZFC AC susceptibility are plotted.
Figure 3: Temperature dependences of ZFC ' (at f = 1 TA is assigned by the hump anomaly in the FC
Hz, on left axis) and M (on right axis) of Co3Sn2S2 at magnetization and ZFC c' and TC is assigned by the
150 Oe applied along the c-axis. The vertical doted lines sharp peak anomaly in the FC magnetization, ZFC c'
indicate TA (see text) and TC. and c". The HT-region surrounded by TA and TC is
3
denoted as the A-phase. In Fig. 5 (a), the saturation 3.4. Relaxation phenomena and frequency
field Hs where the magnetization collapses to the dependence of c' and c".
high-field-limit magnetization is also plotted. It
The existence of a non-zero c" in the A-phase,
should be noted that Hs(T) merges the high-field
particularly around TC and TA, as indicated in sec. 3.2,
boundary of TA(H), which suggests the A-phase is
implies that the spin dynamics slows down to the
characterized by a non-trivial spin texture before
experimental window of f. To see the slow spin
collinear ferromagnetic state is stabilized by
dynamics in the A-phase in detail, the frequency
magnetic field.
dependence of the AC susceptibility of Co3Sn2S2 is
Figure 5 (b) illustrates the HT phase diagram
shown in details in Fig. 6 at temperatures below and
in the case of applied magnetic field perpendicular to
in the A-phase.
the c-axis. The A-phase boundary is not closed
The ZFC c' and c" at several temperatures
because the magnetization dose not saturate in this
under H = 150 Oe are displayed in Figs. 6 (a) and
field direction due to the high magnetic anisotropy.

Figure 4: Thermal variation of ZFC and FC ' and " of Co3Sn2S2 measured at different frequencies from 1 to 1000
Hz and for magnetic fields H of zero (a),(b), 150 Oe (c),(d), and 600 Oe (e),(f), applied along the c-axis. The arrows
indicate TC and TA (see text). For clarity purpose, the data with frequencies of 1, 10 and 100 Hz have been shifted
vertically with respect to the baseline by multiplying their data to the numbers indicated as in (a) and (b).

4
Figure 5: Magnetic H-T phase diagrams of Co3Sn2S2 for fields applied (a) along and (b) perpendicular to the c-axis.
Dashed and solid lines are for the eye guidance.

(b). c' below and around TA are weakly frequency- and c" at TC do not change significantly, indicating
dependent, and correspondingly, c" are almost absent. weak variation of the time scale of spin dynamics
The increased value of c", below TA, at high f can be with increasing of H at TC. Both c' and c" are only
ascribed as an indication of f-dependence at higher f, suppressed with approaching the high field boundary
that was found only in the MHz range in of the A-phase, ~ 250 Oe. Above this field, both c'
ferromagnetic materials31, or likely is an extrinsic and c" are very small and almost frequency-
effect due to eddy currents at low temperatures. independent. It can be interpreted as that spins are
While the boundary from the FM to A-phase at TA is fixed along the field-direction more and more and the
considered by the hump-like anomaly of c', described number of slowly fluctuating spins is reduced by
in sec. 3.2, it is not detectable The frequency magnetic field.
dependence of c' and c" becomes more. The To reveal an overview of the development of
featureless c' and c" are seen until 135 K, where the spin dynamics in the A-phase, phenomenological
minimum is found. At 160 K, deeper inside the A- Cole-Cole formalism that includes a distribution of
phase, c' and c" exhibit pronounced frequency- spin relaxation times32,33 is employed. In the Cole-
dependence. c" strongly increases down to 0.5 Hz, Cole analysis, the AC susceptibility is given by:
'(
indicating the longer time-scale of spin dynamics = +
) + ,-. /01
, (1)
(
than 2 s at 160 K. with A0 = (0) (), where (0) and () are the
The frequency dependence of c' and c" isothermal and adiabatic susceptibilities, = 2f is
becomes more pronounced with approaching to the the angular frequency and is a parameter that
high-temperature boundary between the A- and provides a measure of the width of the distribution of
paramagnetic phases as shown in Figs. 6(c) and (d). the relaxation time. = 0 reverts Eq. (1) to the
It is clearly found that the time-scale of spin dynamics conventional Debye relaxation with a single
becomes shorter with T-increasing and exceeds the relaxation time and = 1 gives an infinite width of
experimental frequency-window at 173 K, above TC. the distribution. The real and imaginary parts of the
The f-dependence of c' and c" at TC, 172 K at H = AC susceptibility can be extracted from Eq. (1) as32
34
0.00 Oe, for different magnetic fields is shown in :
Figs. 6(e) and (f). The frequency dependences of c'

5
'( [) + -.( /01 456(89/;)] clear deviations from the Cole-Cole formalism at low
2 = + >1 , (2)
) + ; -.( /01 456 + -.( ? /01
? frequency for T- and H-regions corresponding to the
22 =
'( -.( /01 @A4(89/;)
, (3) A-phase as seen in Figs. 6 (d) and (f). It indicates
>1
) + ; -.( /01 456 + -.( ? /01
? more complicated dynamics in the A-phase.
The fitting results to Eqs. (2), (3) just in the vicinity 4. Discussion
of TC are shown as solid curves in Figs. 6(c), (e), (d)
and (f). The fitting parameters are shown as functions The magnetization and AC susceptibility
indicate a zero- and low-field characteristic magnetic
of temperature at 150 Oe and as functions on the
transitions to nontrivial spin state just below TC. The
applied field at 172 K in the insets of Figs. 6(d) and
magnetic relaxation process of characteristic
(f), respectively. An estimated little varying at
relaxation times of several seconds at around
around 0.6 against T and H indicates a significant
boarders of the anomalous A-phase and longer inside
distribution of relaxation times. and its weak
indicates a frozen phase. The slow spin dynamics in
variation against T and H. On the other hand, the
the A-phase can be initially ascribed to a glassy spin
characteristic frequency, f0, = 1/t0 varies. Especially,
state35. However, the excluded disorder in our system
f0 drastically decreases with decreasing temperature
and moreover the ferromagnetic order of fast
at around TC, i.e. f0 ~ 25Hz, at 172 K, and f0 ~ 0.1 Hz
relaxation of few microseconds below the anomalies
at 171 K, and lower f0 is observed for T = 170K. The
transition temperatures, TA, indicates the absence of a
variation of f0 at TC against H is more gentle, as seen
glassy state of spins. Given the arrangement of Co
in the inset of Fig. 6(f).
atoms of Co3Sn2S2 in kagom sublattices in its 2D
Actually it should be noted that an
metallic layers, another spin state that results in these
asymmetric bell-shaped f-dependence of c" shows
slow

Figure 6: Frequency dependences of ZFC-' and " of Co3Sn2S2 at T = 50 - 160 K shown in (a), (b) and at 170-172 K
(close to TC) shown in (c), (d), under a magnetic field of 150 Oe applied along the c-axis. (e) and (f) show ZFC-' and
" at TC ~ 172 K for different fields up to 250 Oe applied along the c-axis.

6
relaxation processes is that of large scale units such competing DM interaction, magnetic biskyrmions are
as magnetic skyrmions. The DM interaction in stabilized by the dipolar interaction which possibly
kagom ferromagnets as well as the spin frustration occurs in Co3Sn2S2. To address these expectations,
exchanges that can be emerged by the enhanced further small-angle neutron scattering (SANS)
fluctuations in the vicinity of TC, as described in sec. experiments, spin-polarized scan tunneling
1, are possible mechanisms of a multi-Q spin state. microscopy (STM) or Lorentz TEM microscopy are
Spin frustration is theoretically expected as a needed to shed light on the bulk nature of the
mechanism of magnetic skyrmions stabilization36. magnetic structures of Co3Sn2S2.
Characteristic anomalous magnetic 5. Conclusion
transitions just below TC have been observed in B20
chiral magnets, FeGe15, MnSi37, Fe0.7Co0.3Si38 and The precise measurement of the low-field
Cu2OSeO334,39 at around the A-phase in these magnetization process of Co3Sn2S2 provides an
materials. The net magnetization as well as the AC approach to the H-T phase diagram. Magnetic
susceptibility are minimal in the A-phase due to its transitions at the boarders of an anomalous pocket, A-
non-coplanar spin structure at spots, i.e. skyrmions of phase, as indicated by the DC magnetization and the
antiparallel spins at the core and the peripheral and AC susceptibility were observed just below the
curled spins in between, in a ferromagnetic magnetic order temperature, TC. The disappearance
background. The quite stable state of magnetic of the anomalous transitions at higher fields suggests
skyrmions exhibits slow spin dynamics and the unconventional spin textures, probably of magnetic
narrow temperature window of f-dependence of skyrmions, different from the ferromagnetic state in
characteristic frequency, f0, in the experiment the A-phase. Frequency-distributed spin relaxation
frequency range at the A-phase borders have been process of characteristic relaxation times of several
previously observed in these skyrmion-hosting seconds have been observed close to the A-phase
materials. The spin relaxation process exhibits a boundary.
relaxation time distribution in the vicinity of TC and Acknowledgement
has been described well by the Cole-Cole M.A.K. would like to thank the Egyptian Ministry of
formalism34,3840. The observation of asymmetrically Higher Education for financial support during his
distributed relaxation times inside the A-phase with study in Kyoto University, Japan. This work was
experimental out-of-phase susceptibility, c" (f), partly supported by Murata scientific foundation.
higher than that of the Cole-Cole formalism support
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*
E-mail: kassem.ahmed.82s@st.kyoto-u.ac.jp or Permanent Address: Department of Physics, Assiut
makassem@aun.edu.eg University, Assiut 71515, Egypt

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