PHYSICAL REVIEW B 102, 104407 (2020)

Stability of Néel-type skyrmion lattice against oblique magnetic fields in GaV4 S8 and GaV4 Se8

B. Gross,1 S. Philipp ,1 K. Geirhos ,2 A. Mehlin,1 S. Bordács,3,4 V. Tsurkan ,2,5 A. Leonov,6

I. Kézsmárki,2 and M. Poggio 1,7
1
Department of Physics, University of Basel, 4056 Basel, Switzerland
2
Experimental Physics V, Center for Electronic Correlations and Magnetism, University of Augsburg, 86159 Augsburg, Germany
3
Department of Physics, Budapest University of Technology and Economics, 1111 Budapest, Hungary
4
Hungarian Academy of Sciences, Premium Postdoctor Program, 1051 Budapest, Hungary
5
Institute of Applied Physics, MD-2028 Chisinau, Republic of Moldova
6
Department of Chemistry, Faculty of Science, Hiroshima University Kagamiyama, Higashi Hiroshima, Hiroshima 739-8526, Japan
7
Swiss Nanoscience Institute, University of Basel, 4056 Basel, Switzerland

(Received 24 June 2020; revised 18 August 2020; accepted 19 August 2020; published 3 September 2020)

Nanometer-scale magnetization configurations known as magnetic skyrmions have mostly been studied in
cubic chiral helimagnets, in which they are Bloch-type and their axes align along the applied magnetic field.
In contrast, the orientation of Néel-type skyrmions is locked to the polar axis of the host material’s underlying
crystal structure. In the lacunar spinels GaV4 S8 and GaV4 Se8 , the Néel-type skyrmion lattice phase exists for
externally applied magnetic fields parallel to this axis and withstands oblique magnetic fields up to some critical
angle. Here, we map out the stability of the skyrmion lattice phase in both crystals as a function of field angle
and magnitude using dynamic cantilever magnetometry. The measured phase diagrams reproduce the major
features predicted by a recent theoretical model, including a reentrant cycloidal phase in GaV4 Se8 . Nonetheless,
we observe a greater robustness of the skyrmion phase to oblique fields, suggesting possible refinements to
the model. Besides identifying transitions between the cycloidal, skyrmion lattice, and ferromagnetic states in
the bulk, we measure additional anomalies in GaV4 Se8 and assign them to magnetic states confined to polar
structural domain walls.

DOI: 10.1103/PhysRevB.102.104407

I. INTRODUCTION a plane containing the radial direction, were observed in bulk

GaV4 S8 , GaV4 Se8 [12,17–22], and GaMo4 S8 [23]. These ma-
The discovery of the nanometer-scale magnetization con-
terials crystallize in the cubic lacunar spinel structure [24–31],
figurations known as magnetic skyrmions [1] has spurred
which becomes polar below ∼45 K and the point symmetry is
renewed interest in noncentrosymmetric magnets. The lack of
reduced from Td to C3v [17,31–33]. Since the magnetic order
inversion symmetry in these crystals gives rise to an asymmet-
develops in the polar phase, these compounds are multifer-
ric exchange coupling, known as the Dzyaloshinskii-Moriya
roic. Furthermore, the skyrmions posses a nontrivial electric
interaction (DMI). Crystal symmetry determines the form of
polarization pattern due to the magnetoelectric effect [31],
the free energy term corresponding to the DMI, which—
which may enable nearly dissipation free manipulation of the
in competition with the spin stiffness—stabilizes modulated
magnetic order by electric fields [32].
spin-textures such as spirals and skyrmions and determines
In addition to obvious differences in the spin texture of
their internal structure [2,3]. Both skyrmion lattices (SkLs) Bloch- and Néel-type skyrmions, the phase diagrams of cubic
[4,5] and isolated skyrmions [6] have now been observed in helimagnets and polar skyrmion hosts are markedly differ-
either bulk or nanostructured noncentrosymmetric crystals. ent. In cubic helimagnets, the term in the magnetic energy
Their topologically protected spin-texture, which is stable corresponding to the DMI has an isotropic form: wDMI =
even at room temperature [7], their nanometer-scale size, and M · (∇ × M). Therefore, the plane of the SkL aligns itself
their easy manipulation via electric currents and fields [8–12] to be nearly perpendicular to the applied magnetic field, irre-
make skyrmions a promising platform for information storage spective of the field’s direction. This isotropic interaction also
and processing applications [13,14]. results in a narrow stability range of for Bloch-type skyrmions
Until recently, most investigations in bulk crystals focused in the vicinity of the magnetic ordering temperature due to
on Bloch-type skyrmions, in which the local magnetization competition with the longitudinal conical phase [1,15]. In
rotates perpendicular to the radial direction moving from the contrast, Cnv (n  3) symmetry only allows an axially sym-
skyrmion core to the far field. This type of skyrmion was metric DMI interaction. Therefore, in polar skyrmion hosts,
observed in chiral cubic helimagnets with B20 structure such modulated magnetic structures with wave vectors perpendic-
as MnSi [1], FeGe [15], or Cu2 OSeO3 [16]. Recently, Néel- ular to the high symmetry, polar axis are favored. In these
type skyrmions, in which the local magnetization rotates in compounds, the orientation of Néel skyrmions is locked to

2469-9950/2020/102(10)/104407(9) 104407-1 ©2020 American Physical Society

B. GROSS et al. PHYSICAL REVIEW B 102, 104407 (2020)

the polar axis rather than the applied magnetic field. Thus,
instead of tilting the plane of the SkL, oblique applied fields
distort the configuration of the Néel skyrmions and displace
their cores [34]. This property has two consequences on the
magnetic phase diagram of such materials: (1) the SkL phase
is more robust than in cubic helimagnets because the conical
phase is suppressed, and (2) its stability range depends on
the direction of the applied field. In addition, the second-
order magnetic anisotropy allowed in this symmetry can also
modify the phase diagram. In the case of GaV4 S8 , strong easy-
axis anisotropy [33] suppresses the modulated phases at low
temperature [19], whereas in GaV4 Se8 easy-plane anisotropy
helps to stabilize the SkL phase down to the lowest tempera-
tures [12,18,20].
Here, we use dynamic cantilever magnetometry (DCM)
[35–37] to map the magnetic phase boundaries in GaV4 S8 and
GaV4 Se8 as a function of the strength and orientation of mag-
netic field. We determine the corresponding phase diagrams,
which reproduce the major features predicted by a recent FIG. 1. Schematics of the measurement setup. (a) The coordinate
theoretical model [34]. The measurements constitute a di- system and the definition of β as the angle between H and x̂ in the
rect experimental confirmation of the robustness of Néel-type top figure. Below, the rotation plane of H and the definition of the
skyrmions to oblique magnetic fields in two materials with angles αi is given. (b), (c) The cantilever, its oscillation angle θc , and
uniaxial magnetic anisotropy of opposite signs. In addition the crystalline axes of the measured samples. Black, red, green, and
to magnetic transitions between the cycloidal, SkL, and field- blue lines correspond to the four ĉi . (d) The orientation of H with
polarized ferromagnetic states, in GaV4 Se8 , we also observe respect to an optical image of a sample and cantilever. (e) Composite
sharp anomalies in the torque, which we assign to field-driven optical and scanning electron micrographs of the measured GaV4 S8
transformations of magnetic states confined to polar domain and GaV4 Se8 samples mounted on their respective cantilevers.
walls (DWs).

the cantilever at f with a constant oscillation amplitude of

II. DYNAMIC CANTILEVER MAGNETOMETRY
a few tens of nanometers (corresponding to oscillation angles
In DCM, the sample under investigation is attached to the of tens of microradians) using a feedback loop implemented
end of a cantilever, which is driven into self-oscillation at its by a field-programmable gate array. This process enables
resonance frequency f . Changes in this resonance frequency the fast and accurate extraction of f from the cantilever
 f = f − f0 are measured as a function of the uniform ap- deflection signal as well as providing a measure of the dis-
plied magnetic field H, where f0 is the resonance frequency at sipation , which described the system’s rate of energy loss:
H = 0.  f reveals the curvature of the magnetic energy Em 2
dE /dt = −le2 θ˙c . To maintain a constant oscillation ampli-
with respect to rotations about the cantilever oscillation axis tude, the cantilever must be driven with a force F = le θ˙c ,
[35,36]: such that any losses due to dissipation are compensated. The
  
f0 ∂ 2 Em  voltage amplitude used to drive the piezoelectric actuator is
f = , (1) therefore proportional to  = 0 + m where 0 is the can-
2k0 le2 ∂θc2 θc =0 tilever’s intrinsic mechanical dissipation at H = 0 and m
where k0 is the cantilever’s spring constant, le its effec- represents magnetic losses. Given that m reflects the sam-
tive length, and θc its angle of oscillation. Measurements of ple’s magnetic relaxation,  should undergo abrupt changes
this magnetic curvature are particularly useful for identifying at magnetic phase transitions. We therefore use both measure-
magnetic phase transitions [35] since—just as the magnetic ments of the magnetic curvature and dissipation, combined
susceptibility—it should be discontinuous for both first- and with knowledge from other measurements [12,17–20], to map
second-order phase transitions [38]. the low-temperature magnetic phase diagrams of GaV4 S8 and
DCM measurements are carried out in a vibration-isolated GaV4 Se8 as a function of H.
closed-cycle cryostat. The pressure in the sample chamber is
less than 10−6 mbar and the temperature can be stabilized
III. SAMPLES
between 4 and 300 K. Using an external rotatable supercon-
ducting magnet, magnetic fields up to 4.5 T can be applied Single crystals of GaV4 S8 and GaV4 Se8 are grown by a
along any direction spanning 120◦ in the plane of cantilever chemical transport reaction method using iodine as a transport
oscillation, as shown in Fig. 1. x̂ in our coordinate system agent [17]. X-ray diffraction measurements of both sample
is defined by the cantilever’s long axis, while ŷ coincides materials show impurity-free single-crystals [31]. For the
with its axis of oscillation. β is the angle between H and DCM measurement, we attach individual crystals of GaV4 S8
x̂ in the xz-plane. The cantilever’s motion is read out using and GaV4 Se8 , which are a few tens of micrometers in size,
a optical fiber interferometer using 100 nW of laser light at to the ends of commercial Si cantilevers (NanosensorsTM TL-
1550 nm [39]. A piezoelectric actuator mechanically drives cont) using nonmagnetic epoxy, as shown in Fig. 1. These

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FIG. 2. Temperature and field dependence of magnetic phase transitions measured by DCM in GaV4 S8 . DCM measurements of (a)  f (H )
and (b) (H ) taken at T = 7, 12, and 15 K in cyan, maroon, and brown, respectively. Curves are shifted for better visibility. β = 0, i.e.,
approximately H  [100]. Arrows indicate features corresponding to phase transitions. (c) Sketch of the expected magnetic phase diagram as
a function of temperature and applied field for H  [100] [17]. Color-coded dashed lines and points correspond to temperatures and measured
features in (a) and (b).

cantilevers are 440-μm-long, 50-μm-wide, and 2.3-μm- along ĉi , making these the polar axes of the system. The
thick. Unloaded, they have resonance frequencies of about multidomain state is composed of sub-micrometer-thick
16 kHz, quality factors around 5 × 105 , and spring constants sheets of these four different rhombohedral polar domains,
of 300 mN/m. Due to the additional mass of the samples, which we label Pi [20,21]. The polar axis ĉi also corresponds
the resonance frequency of a loaded cantilever shifts to to the axis of magnetic anisotropy in the respective
around 3 kHz. rhombohedral domain state. In GaV4 S8 , the uniaxial
Both samples are attached near the free end of the can- anisotropy is of easy-axis type, while in GaV4 Se8 it is of
tilever with the (001) surface pressed flat against the Si easy-plane type [17,18,33]. In both materials, measurements
surface. The orientation of the GaV4 S8 and GaV4 Se8 samples indicate the presence of modulated magnetic phases including
differs and can be roughly estimated from optical and scan- a cycloidal (Cyc) state, a Néel-type SkL, and a field-polarized
ning electron microscope images. The resultant direction of ferromagnetic (FM) phase [17,18]. The population of multiple
each sample’s crystalline axes with respect to the cantilever rhombohedral domains at low temperature complicates the
is shown in Fig. 1: specifically the approximate orientation of determination of the magnetic phase diagram because, for
the four cubic 111 axes ĉi (i = 1, 2, 3, 4) is shown in black, any given orientation of the applied field H, there can be up
red, green, and blue. to four different angles, αi , between H and ĉi as shown in
Both GaV4 S8 and GaV4 Se8 undergo a Jahn-Teller Fig. 1(a). Note that we define αi modulo 180◦ ; due to crystal
structural phase transition from a noncentrosymmetric cubic symmetry, if αi exceeds 180◦ , the relevant angle is between
to a rhombohedral structure at 44 and 42 K, respectively H and −ĉi . As a result of the four possible αi , for an arbitrary
[11,12,30,31]. The transition is characterized by a stretching orientation of H, a single phase transition can appear at up to
of the cubic unit cell along one of the four cubic body four different values of H, depending on the projections of H
diagonals ĉi , resulting in four different structural domains. on each ĉi . Although the application of a large electric field
The rhombohedral distortion also gives rise to polarization upon cooling through the structural phase transition has been

FIG. 3. Angular dependence of magnetic phase transitions measured by DCM in GaV4 S8 . (a), (b)  f (H ) at T = 11 K for at β = 0, 40,
and 90◦ in maroon, cyan, and brown, respectively. Arrows indicate features corresponding to phase transitions. Inset: Zoomed view of the
low-field region. (c) Schematic diagram showing the three measured orientations relative to the sample-loaded cantilever.

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B. GROSS et al. PHYSICAL REVIEW B 102, 104407 (2020)

shown to polarize GaV4 S8 and GaV4 Se8 samples such that

400 (a)
only a single domain is populated [11,12], it is practically

H (mT)
challenging to apply such fields in a DCM apparatus.
300
200
IV. MEASUREMENTS

0
A. GaV4 S8 100
Figure 2 shows DCM measurements of  f (H ) and (H )
in GaV4 S8 for different temperatures T . The data shown in 0
400 (b)
Figs. 2(a) and 2(b) are collected with H aligned along the
cantilever’s long axis (β = 0), i.e., approximately H  [100].

H (mT)
In this configuration, the angles αi between H and the four ĉi
300
are the same within the precision of the sample orientation,
i.e., within a few degrees. Consequently, each magnetic phase
200

0
transition should occur at a similar value of H for each do-
main. In this particularly simple case, we compare  f (H ) and 100
(H ) at different temperatures to the corresponding magnetic
phase diagram measured by Kézsmárki et al. [17] and shown 0
75 (c)

(°)
schematically in Fig. 2(c). Where metamagnetic transitions
are expected, they manifest themselves as dips in  f (H ) 50

i
and peaks in (H ). At T = 12 K, the two features at 45 and 25
100 mT (indicated by arrows) correspond to the Cyc-to-SkL 0
and the SkL-to-FM phase transitions, respectively. The double 0 10 20 30 40 50 60 70 80 90
dip (peak) feature in  f (H ) [(H )] comes from the imperfect (°)
alignment of the sample’s crystalline axes with the coordinate
(d) GaV 4 S 8
system of our measurement setup, resulting in a difference in
αi for each domain. At T = 7 K only one feature is found, cor-
300 T = 11 K
responding to the Cyc-to-FM transition, while at T = 15 K,
H|| (mT)

which is above the magnetic ordering temperature, no features FM

are observed. 200
H is rotated approximately in the (010) plane such that,
in general, by changing β, we change each αi differently. As
0

a result, the number of features related to phase transitions

and the fields at which they occur can also change. The de- 100 = 79°
p
pendence that we observe is consistent with the orientation of max ex
our sample and previous measurements by Kézsmárki et al. SkL
In particular, we note that, because of the crystal’s alignment
Cyc
0
and its cubic symmetry, the measured curves should repeat 0 100 200 300 400
themselves upon rotating β by 90◦ . This periodic behavior
0
H (mT)
can be seen in Fig. 3(a), where two DCM curves with β = 0
and 90◦ nearly overlap; differences, including the splitting
FIG. 4. Magnetic phase transitions measured in GaV4 S8 at T =
of the dips in  f (H ) into two dips, are again related to
11 K. Features extracted from DCM measurement of (a)  f (H )
the slight misalignment of the sample’s crystalline axes with
and (b) (H ) are plotted as open circles as a function of β. Black,
respect to the applied field, resulting in slightly different αi for red, green, and blue circles correspond to domains P1 , P2 , P3 , and
each domain. In the curve taken with β = 40◦ (approximately P4 , respectively. Color-coded lines indicate phase boundaries for
H  [101]) shown in Fig. 3(b), we observe four features. The each domain according to the phase diagram in (d). (c) Angle αi
features observed at 26 and 68 mT are the Cyc-to-SkL and the between the corresponding ĉi and the external field H vs β for all
SkL-to-FM phase transitions, respectively, also observed by four rhombohedral domains, using the same color code as in (a) and
Kézsmárki et al. These transitions correspond to the P4 and P1 (b). (d) Best-fit magnetic phase diagram for single-domain GaV4 S8
domains (blue and black in Fig. 1) with α4 = 31.7◦ and α1 = as a function of field applied perpendicular and parallel to the axis of
39.2◦ . The two transitions at 320 and 370 mT correspond to symmetry.
the Cyc-to-FM transitions in the P3 and P2 domains (green and
red in Fig. 1), where α3 = 84.5◦ and α2 = 88.8◦ . As before,
the mismatches α4 = α1 and α3 = α2 and the resulting pair of H = 1 T, DCM measurements are made by stepping H toward
split features are due to the crystal’s imperfect alignment with zero at a fixed β and T . The angular dependence over the
the applied field. range −5◦ < β < 100◦ is recorded at T = 11 K by changing
Using the measured features in  f (H ) and (H ), we map β in steps of 2.5◦ and repeating the measurement. We plot
the magnetic phase transitions of GaV4 S8 as a function of H the features identified in these measurements as open circles
and β. After initializing the system with a large external field in Figs. 4(a) and 4(b). By comparing our data taken for a

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1°
(a)

6.6
300 (d)

=3
300

=2
H (mT)

xp
H|| (mT)

xe
i
200

ma
200 SkL FM
0

100

0
100
0 Cyc GaV 4 Se 8
(b) T = 12 K
300 0
0 100 200 300 400
H (mT)

0
H (mT)
200 10
(e)
8
0

(a.u.)
Cyc SkL Cyc FM
100
6
0 4

f (Hz) /
75 (c)
2
(°)

50 0
i

25
-2 i
= 26.6°
0
0 25 50 75 100 125 150 175 200 0 100 200 300
(°) 0
H (mT)

FIG. 5. Magnetic phase transitions measured in GaV4 Se8 at T = 12 K. Transitions extracted from DCM measurement of (a)  f (H ) and
(b) (H ) are plotted as open circles as a function of β. Black, red, green, and blue circles correspond to transitions for domain P1 , P2 , P3 , and
P4 , respectively. Color-coded lines correspond to phase boundaries for the each color-coded domain as indicated by lines in the phase diagram
(d). (c) Angle αi between corresponding polar axis and the external field H vs β for all four rhombohedral domains, using the same color
code as in (a) and (b). (d) Best-fit magnetic phase diagram for single-domain GaV4 Se8 as a function of field applied perpendicular and parallel
to the axis of symmetry. (e) DCM measurement of  f (H ) for αi = 26.6◦ (β = 7.5◦ ) showing the reentrant Cyc phase of domain 1 (black).
Transitions from other domains are not indicated. These measurements corresponds to line-cuts along the dotted vertical lines in (a) and (b) and
the dotted diagonal line labeled αi = 26.6◦ in (d).

few magnetic field orientations to the phase diagram reported to ideal configuration, shown in Fig. 1(b), is required such that
by Kézsmárki et al. [17], we assign each feature to a certain the phase boundaries corresponding to the different domain
type of transition (i.e., Cyc-to-FM, Cyc-to-SkL, SkL-to-FM) states collapse onto the single boundary diagram of Fig. 4(d).
occurring in a certain domain state (P1 , P2 , P3 , P4 ). Note that features shown in Figs. 4(a) and 4(b) related to the
Next, we determine the dependence of the phase bound- Cyc-to-FM transitions of P1 (black) and P4 (blue) are very
aries on the orientation of the magnetic field with respect to weak in  f (H ) and not observable in (H ). Given that we
the axis of the uniaxial magnetic anisotropy. The measured cannot control the population of the domains, it is likely that
signatures shown as open circles in Figs. 4(a) and 4(b) can the sample is in a multidomain state dominated by P2 (red)
be fit by assuming that each of the four rhombohedral do- and P3 (green) domains.
mains of GaV4 S8 obeys the magnetic phase diagram shown in The agreement between the measured features and fit phase
Fig. 4(d), plotted as a function of H and H⊥ , the components boundaries allows us to eliminate complications arising from
of H parallel and perpendicular to the rhombohedral axis ĉi , the multidomain nature of the crystal and, thus, to extract a the
respectively. A feature in  f and  observed at certain H general magnetic phase diagram of GaV4 S8 as a function of
and β corresponds to a transition of a particular domain Pi the field applied parallel and perpendicular to the anisotropy
for a field of magnitude H and angle αi with respect to ĉi , as axis. The position of the intersection between the different
shown in Fig. 4(c). The magnitude H and the angle αi at which phase transitions in Fig. 4(d) shows that the SkL phase in
each feature occurs, correspond to a point on a phase bound- GaV4 S8 persists in oblique fields up to a threshold angle as
ary in the diagram of Fig. 4(d), through H = H cos αi and large as αmax = 79◦ . For larger α, the cycloidal state directly
H⊥ = H sin αi . This phase diagram reflects the general form transforms to the ferromagnetic state upon increasing H. The
suggested by Leonov and Kézsmárki [34]. Phase boundaries extent of the SkL phase shows stronger stability against fields
corresponding to the diagram are also plotted as a function applied perpendicular to the anisotropy axis (up to H⊥ =
of β and H in Figs. 4(a) and 4(b) to show their agreement 200 mT) than fields applied parallel (up to H = 65 mT). The
with the measurements. They appear as solid lines, which are critical angle αmax is larger than predicted by Leonov and
color-coded according to the domain to which they belong. A Kézsmárki [34], although their model was not designed for
Euler rotation of the crystal (−5.0, 0.2 and 10.0◦ ) with respect strict quantitative comparisons.

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Note that the rotation plane of H, approximately (11̄0), con-

tains ĉ1 and ĉ2 , but not ĉ3 and ĉ4 . A Euler rotation of the crystal
(−14, −1, and 7◦ ) with respect to the ideal configuration,
shown in Fig. 1(c), is required such that the phase bound-
aries corresponding to the different domain states (P1 , P2 , P3 ,
P4 ) collapse onto the single boundary diagram of Fig. 5(d).
We find additional anomalies in both  f (H ) and (H ) that
cannot be ascribed to the boundaries between the Cyc, SkL,
and FM phases. We suspect that these anomalies originate
from the formation of magnetic textures localized at structural
DWs, as discussed in Sec. IV C.
Features assigned to the Cyc-to-FM transition of domain P3
(green) are difficult to distinguish from those occuring for the
same transition in P4 (blue) because they are expected to occur
at nearly the same H and β in Figs. 5(a) and 5(b). Since this
distinction does not affect the form of the phase diagram in
Fig. 5(d), our assignment of all such features to the P3 rather
than P4 transition is unimportant. For the P1 (black) and P2
(red) domains, which are the only two experiencing sufficient
H to reach the SkL phase, the boundaries of the SkL state
FIG. 6. Schematic for understanding the orientation of the 6 dif- appear as prominent rain-drop-like shapes in Figs. 5(a) and
ferent domain walls types. Top left: Directions of the four possible
5(b). From the intersection of the SkL with the Cyc phase
polar axes, P1 -P4 , which are the axes of magnetic anisotropy within
boundary in Fig. 5(d), we extract a threshold angle αmax = 31◦
the corresponding domains. The transparent blue plane indicates the
for the SkL phase in GaV4 Se8 at T = 12 K. Contrary to
approximate plane of rotation of the external magnetic field. Top
right: Mechanically compatible and charge neutral DWs separating
GaV4 S8 , the extent of the SkL phase shows stronger stability
P1 and P2 domains are parallel to the (001) plane, just as DWs against fields applied parallel to the anisotropy axis (up to
between P3 and P4 domains. The former and latter DWs are referred H = 340 mT) than fields applied perpendicular (up to H⊥ =
to as P1 P2 and P3 P4 , respectively. γn , the angle between H and the 75 mT). Furthermore, we note the presence of a reentrant Cyc
normal vector n, which is proportional to ĉi + ĉ j , is shown for both phase for angles 19◦ < αi < 30◦ , as predicted by Leonov and
DW pairs. γ p , the angle between H and ĉi − ĉ j , is also shown. Kézsmárki [34]. For this range of αi , two successive first-
Bottom: The other two pairs of DWs sharing the same orientation. order phase transitions from Cyc to SkL and back occur as
The normal vector of the corresponding planes and their labels are a function of increasing field. The signature of this behavior
indicated for the three cases, as well as the difference vector ĉi − ĉ j , in DCM is shown in Fig. 5(e).
unique to each DW type.
C. Magnetic states confined to domain walls in GaV4 Se8
Geirhos et al. observed anomalies in various macroscopic
B. GaV4 Se8 thermodynamic properties of GaV4 Se8 , emerging exclusively
We apply the same experimental procedure to explore the in crystals with polar multidomain structure. They suggest a
magnetic phase diagram of GaV4 Se8 . In this case, H is rotated possible scenario for the formation of magnetic states at the
approximately in the (11̄0) plane. Figs. 5(a) and 5(b) show structural DWs [20]. Magnetic interactions change stepwise
the angular dependence of the features, as extracted from at the DWs, where spin textures with different spiral planes,
measurements of  f (H ) and (H ) at T = 12 K. Using pre- hosted by neighboring domains, need to be matched. This
vious measurements made by Bordács et al. along particular can, for example, lead to conical magnetic states at the DWs
crystalline directions [18], as well as neutron diffraction data with a different closing field magnitude than bulk magnetic
by Geirhos et al. [20] for guidance, we assign each feature states. Here, we adopt and modify this model in order to
to a transition between Cyc, SkL, or FM states for a certain analyze its applicability to anomalies observed in our DCM
domain and color-code it accordingly. measurements of GaV4 Se8 , which cannot be assigned to bulk
Once again, the measured features are shown as open cir- magnetic phase transitions.
cles in Figs. 5(a) and 5(b) and can be fit by assuming that each In the rhombohedral phase of the studied lacunar spinels,
of the four rhombohedral domains obeys a single magnetic mechanically compatible and charge-neutral DWs are normal
phase diagram shown in Fig. 5(d). The magnitude of the to ĉi + ĉ j , the sum of the two polar directions of the domain
applied field H and its angle αi with respect to the assigned states Pi and Pj separated by the DW, as shown in Fig. 6
domain’s rhombohedral axis ĉi put each feature on one of [20,21,40]. For example, mechanically and electrically com-
the phase boundaries depicted in Fig. 5(d). Phase boundaries patible DWs connecting a P1 (black) and a P2 (red) domain are
corresponding to the phase diagram are plotted in Figs. 5(a) parallel to (001) planes, cf., Fig. 6. The same is true for DWs
and 5(b) for comparison to the measured data. They appear between P3 (green) and P4 (blue) domains.
as solid lines, which are color-coded according to the domain. For an arbitrary orientation of the external magnetic field,
Similarly to GaV4 S8 , the overall form of the phase diagram magnetic states confined to DWs with different orientations
agrees with that suggested by Leonov and Kézsmárki [34]. are expected to undergo field-induced transitions, similarly to

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FIG. 7. Anomalies in  f (H ) and (H ) assigned to transitions of DW rather than bulk magnetic states. Arrows at the top indicate from
left to right the approximate angle β corresponding to the [111], [001], and [11 − 1] directions, respectively. (a) Angle γn between the normal
vector of a DW and H plotted against β. The color of the dashed lines shows their correspondence to a DW type in the legend. (b) Angle
γ p between the vector formed by the difference of the polar axis vectors of the two adjacent domains of a DW and H plotted against β.
(c) Transitions extracted from both  f and  that are not assigned to a domain transition (circles). Crosses show transitions extracted from
magnetoelectric measurements [20], scaled by about 0.9 to match the DCM data. Colored lines show the suggested assignment of the transitions
to DW types as denoted in the legend. Light gray lines show the bulk domain transitions. (d) Same data as in (c) with a different assignment of
transitions. Color map of (e)  f (H, β ) and (f) − log10 (H, β ). (g), (h) Example DCM measurements with dash-dotted vertical lines indicating
the assigned transition fields. Dash-dotted vertical lines in (c) indicate the value of β of the example measurements.

the bulk (in-domain) magnetic states. However, in this case in Fig. 6, each sharing the same γn for a given H. For DWs in
the situation is more complex: The stability of the magnetic a pair, however, the relative orientation between the magnetic
states confined to DWs is determined by the orientation of the anisotropy axes of the two domains involved and H is not the
field with respect to the magnetic anisotropy axes of adjacent same. For example, consider the P1 P2 /P3 P4 pair: the rotation
domains and to the DW itself. plane of H (11̄0) contains the anisotropy axes of P1 and P2 ,
It is reasonable to assume that the angle γn between H and but not the anisotropy axes of P3 and P4 ; they span 54◦ with
the normal of the DW planes, given by ĉi + ĉ j , plays a deci- this plane. We therefore introduce another angle γ p between H
sive role in setting the angular range, across which confined and the difference of the two polar vectors ĉi − ĉ j , which lies
states are stable. This leads to three pairs of DWs, as shown in the DW plane. Both these angles γn (β ) and γ p (β ), plotted

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in Figs. 7(a) and 7(b), respectively, are expected to affect the theoretical predictions of Leonov and Kézsmárki [34], con-
stability of the DW-confined magnetic states. firming the general validity of their model. This agreement,
In the angular dependent torque measurements, shown in in turn, provides indirect confirmation that, under oblique
Figs. 7(c) to 7(f), we observe at most four anomalies (open applied magnetic field, the axes of Néel-type skyrmions stay
circles) for a given field orientation. Since there are six types locked to the anisotropy axis while their structure distorts and
of DWs, distinguished by γn and γ p , some transitions, which their core displaces. The measurements reproduce the overall
occur simultaneously in different types of DWs appear as a structure of the phase diagrams, imposing a maximum angle
single anomaly, while some transitions appear not to be exper- αmax of magnetic field applied with respect to the anisotropy
imentally observable. In the following analysis, we take into axis, for which a SkL phase persists. In addition, they show
account an additional anomaly (crosses) between β 40 and that easy-axis anisotropy—as found in GaV4 S8 —enhances
130◦ at field values around 100 mT, which is not present in our the robustness of Néel skyrmions against magnetic fields ap-
DCM measurements, but has been observed in magnetoelec- plied perpendicular to the symmetry axis, while easy-plane
tric measurements [20]. Example measurements of  f and  anisotropy—as found in GaV4 Se8 —increases their stability
are shown in Figs. 7(g) and 7(h), where anomalies assigned to for fields parallel to this axis. Our results also confirm the
DW states are indicated by vertical dash-dotted lines. existence of a reentrant Cyc phase in GaV4 Se8 , which was an-
As a first scenario, we suggest the assignment of the ob- ticipated to occur for certain values of easy-plane anisotropy.
served anomalies as shown in Fig. 7(c). In this way, both Finally, anomalies in  f (H ) and (H ), which cannot be ex-
domains adjacent to a DW host the Cyc state and the DW- plained as bulk domain transitions, are consistent with distinct
confined state emerges due to the matching of these two magnetic states confined to polar structural DWs and their
cycloidal patterns for all observed anomalies. This is specif- transition from the Cyc to FM state, as proposed by Geirhos
ically notable for the anomalies meeting at β ≈ 90◦ . For et al. [20].
example, the anomaly assigned to be a P2 P4 DW (orange), Nevertheless, the measured magnetic phase diagrams are
would progress above 150 mT for β > 90◦ , but because in- not in strict quantitative agreement with the predicted ones.
domain states within the P4 domain (blue axis) transform For GaV4 S8 , we are unable to tune the uniaxial anisotropy of
from the Cyc to the FM state for β > 90◦ and H > 150 mT, the model to match the measured values of threshold angle
this anomaly disappears for larger angles. The same is true of the SkL phase αmax = 79◦ at T = 11 K. This discrep-
for the other end of this anomaly (β = 12.5◦ ). Similarly, the ancy suggests that approximations made in the model ignore
anomalies assigned to transitions in the P1 P2 DWs are limited important details, thus preventing it from capturing the full
by the two skyrmion pockets of the P1 and P2 domains. No behavior of the system. Possible improvements to the model
anomaly is observed in angular ranges, where the adjacent include consideration of the anisotropic exchange interaction,
domains host magnetic states other than the Cyc. an extension from two to three dimensions, or the considera-
An alternative scenario is an extension of the one suggested tion of metatable magnetic states. Also, further experimental
by Geirhos et al. [20], shown in Fig. 7(d). This scenario investigation—especially real-space imaging—of anomalies
allows some DW transitions to persist even when one of the assigned to transitions of DW-confined magnetic states is
adjacent domains is in the Cyc phase, while the other one required to characterize the spin pattern associated with these
is in the SkL phase. Such a situation occurs for the P1 P2 states.
DW transition, which penetrates both the P1 and the P2 SkL
pockets. ACKNOWLEDGMENTS
In both scenarios, the mirror symmetry expected across We thank Sascha Martin and his team in the machine shop
β 90◦ , as dictated by γn (β ) and γ p (β ) is fulfilled: the tran- of the Physics Department at the University of Basel for
sition lines are either symmetric to this point or they have a help building the measurement system. We acknowledge the
symmetry-related counterpart. The basis for both scenarios support of the Canton Aargau and the Swiss National Science
is the occurrence of a distinct magnetic state confined to Foundation under Project Grant 200020-159893, via the Sin-
DWs, and its transition to the FM state at certain critical field, ergia Grant “Nanoskyrmionics” (Grant No. CRSII5-171003),
observed as an additional anomaly in the DCM measurement. and via the NCCR “Quantum Science and Technology”
The angle of the applied field with the DW-normal, γn , and (QSIT). We further acknowledge the support of the BME
the orientation of its component in the DW-plane, γ p , appear Nanotechnology and Materials Science TKP2020 IE grant of
to be a important parameters in determining the critical field NKFIH Hungary (BME IE-NAT TKP2020), the Hungarian
of the DW states. National Research, Development, and Innovation Office-
NKFIH via Grant No. ANN 122879. This research was partly
funded by Deutsche Forschungsgemeinschaft (DFG) via the
Priority Program SPP2137, Skyrmionics, under Grant Nos.
V. CONCLUSION
KE 2370/1-1, via the Transregional Collaborative Research
We extract magnetic phase diagrams as a function ap- Center TRR 80 “From Electronic correlations to functional-
plied field magnitude and direction for both GaV4 S8 and ity” (Augsburg, Munich, Stuttgart), and by the project ANCD
GaV4 Se8 that are in good qualitative agreement with the 20.80009.5007.19 (Moldova).

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