PHYSICAL REVIEW LETTERS 122, 057206 (2019)

Anomalous Nonreciprocal Electrical Transport on Chiral Magnetic Order

Ryuya Aoki,1 Yusuke Kousaka,2 and Yoshihiko Togawa1
1
Department of Physics and Electronics, Osaka Prefecture University, 1-1 Gakuencho, Sakai, Osaka 599-8531, Japan
2
Research Institute for Interdisciplinary Science, Okayama University, Okayama, Okayama 700-8530, Japan

(Received 5 September 2018; published 8 February 2019)

Nonreciprocal flow of conduction electrons is systematically investigated in a monoaxial chiral

helimagnet CrNb3 S6 . We found that such directional dichroism of the electrical transport phenomena,
called the electrical magnetochiral (EMC) effect, occurs in a wide range of magnetic fields and
temperatures. The EMC signal turns out to be considerably enhanced below the magnetic ordering
temperature, suggesting a strong influence of the chiral magnetic order on this anomalous EMC transport
property. The EMC coefficients are separately evaluated in terms of crystalline and magnetic contributions
in the magnetic phase diagram.

DOI: 10.1103/PhysRevLett.122.057206

Chiral structures play an important role in inducing a the chiral magnetic order [24,25], as exemplified by
variety of striking physical responses. For instance, optical discrete magnetoresistance (MR) [26] or topological Hall
rotation and circular dichroism occur in chiral media being effect [27]. In this respect, it is quite interesting to learn how
illuminated by polarized electromagnetic (EM) waves. the chiral magnetic order influences nonreciprocal transport
Recently, in addition to a natural optical activity, directional phenomena.
dichroism, in which the absorption of incident EM waves The EMC effect was recently investigated in a cubic
differs when reversing a propagation direction of the EM chiral helimagnet MnSi which contains multiple helical
waves in the presence of a magnetic field, has attracted axes and may allow the formation of domain structures of
considerable interest. Indeed, this remarkable phenomenon the chiral magnetic order [14]. It was reported that the EMC
has been observed in a range of frequencies of the EM
waves including visible light [1–3], x ray [4], and micro-
wave [5,6]. Such directional dichroism or nonreciprocal
response has also been discussed in transport phenomena of
quasiparticles such as magnons [7,8] and phonons [9] in
noncentrosymmetric crystals under the influence of a
magnetic field.
Nonreciprocal transport of conduction electrons, fre-
quently called the electrical magnetochiral (EMC) effect
[10–16], is phenomenologically expressed by

RðH; IÞ ¼ R0 ð1 þ γμ0 H · IÞ: ð1Þ

The second term on the right-hand side corresponds to the

EMC resistance REMC and indicates an electrical resistance
dependent on the directions of the external magnetic field
H and electric current I. Here, γ is the REMC coefficient and
its sign is associated with structural chirality. The magni- FIG. 1. Schematics of the EMC effect (a), chiral magnetic order
tude of REMC alters in accordance with four combinations (b), and a crystal structure of CrNb3 S6 (c). Nonreciprocal flow of
of H and I directions when both orient toward the helical conduction electrons occurs along the helical axis in the presence
axis, as schematically drawn in Fig. 1(a). of H. The EMC resistance amplitude varies depending on the
directions of H and I, respectively indicated by red and yellow
Chiral helimagnetic materials can host topological spin
bold arrows, with respect to the helical axis (black thin arrow).
structures such as chiral helimagnetic order [17,18], chiral The change in the electric current amplitude occurs when
conical structure, chiral soliton lattice (CSL) [19,20], and measuring the EMC resistance with the constant voltage applied,
chiral magnetic skyrmions [21–23], as partially illustrated as schematically illustrated by the size of yellow arrows in (a).
in Fig. 1(b). Importantly, nontrivial transport phenomena Alternatively, the EMC voltage changes are detected with the
are induced through the coupling of itinerant electrons with current amplitude fixed in this study.

0031-9007=19=122(5)=057206(6) 057206-1 © 2019 American Physical Society

 PHYSICAL REVIEW LETTERS 122, 057206 (2019)

signal is enhanced at large fields above the critical temper- the sample by using electron beam lithography and liftoff
ature T c . This enhancement is ascribed to chiral spin techniques. The critical temperature is determined to be
fluctuations induced in a crossover region between the 121 K by the electrical resistance measurements, which
paramagnetic (PM) phase and the forced ferromagnetic also provided field and temperature information regarding
(FM) phase. However, the EMC intensity appears to be the phase boundaries among the PM, forced FM, and chiral
significantly suppressed at low magnetic fields and temper- conical phases [31].
atures where the chiral conical phase and chiral magnetic When an ac current I ¼ I 0 sinωt is applied to the sample,
skyrmions are predominantly formed. Thus, the contribu- a nonlinear EMC voltage is induced, as expressed by
tion of the chiral magnetic order to the EMC effect was not
clear in the previous experiment.   
γ π
In this Letter, the nonreciprocal EMC transport proper- V EMC ðtÞ ¼ IREMC ¼ μ0 R0 I 20 H 1 − sin 2ωt þ : ð2Þ
2 2
ties are investigated in a prototype monoaxial chiral
helimagnet CrNb3 S6 . We revealed that drastic changes
of the EMC response are driven upon the formation of the The second harmonic resistance R2ω was measured in order
chiral magnetic order. The EMC signal is considerably to detect the REMC using a lock-in technique with an ac
enhanced in the chiral conical phase and the REMC takes its current whose frequency was 13 Hz. The maximum
maximum absolute value just below T c. The crystalline and amplitude of the current was set to 4.5 mA, corresponding
magnetic counterparts of the EMC response are separately to a current density of 1.1 × 109 A=m2 . The Joule heating
detected in a wide range of magnetic fields and temper- effect was negligibly small at this value.
atures. The magnetic term turns out to be about 3 orders of The measurements were performed as a function of the
magnitude larger than the crystalline term, thereby causing applied magnetic field at various temperatures in a con-
the anomalous EMC response on the chiral magnetic order. figuration where H and I were parallel to the c axis, as
The monoaxial chiral helimagnet CrNb3 S6 has a crystal shown in Fig. 1(a). The angular dependence of R2ω was
structure consisting of hexagonal planes of NbS2 and also examined by changing the H direction within the
intercalated Cr atoms, as illustrated in Fig. 1(c). It belongs sample plane with regards to the c axis. During the
to the space group P63 22. The principal (c) axis of the measurements, it was confirmed that the R2ω exhibited
crystal is coincident with the single helimagnetic axis π=2 phase shift against the first harmonic input. The
observed in this compound. measured R2ω showed a field-dependent behavior and
The magnetic phase diagram of CrNb3 S6 consists of the contained both even and odd components with regards
CSL and chiral conical phases. Advantageously, only the to zero magnetic field. The former was the background
chiral conical phase emerges without accompanying any derived from asymmetry of the electrode geometry, while
domain structure and hysteresis effect in magnetic fields the latter was ascribed to the REMC signal as presented in
applied in the direction parallel to the c axis [28]. In the following. More precisely, the REMC signal was
addition, the CSL, which appears in magnetic fields applied obtained by calculating ½R2ω ðH; IÞ − R2ω ð−H; IÞ=2.
perpendicular to the c axis, makes no contribution to the Figure 2(a) shows the calculated data as a function of H
EMC signal because it has magnetic moments rotating only above T c . A linear dependence of the signal on the field
within the ab plane and induces no effective field along the strength is clearly observed at 200 K, which is consistent
c axis. Thus, the CSL will work as an ideal reference state with the behavior expected for the REMC of chiral non-
to the chiral conical phase when studying the EMC effect. magnetic materials [10,12] and indicates the high quality of
CrNb3 S6 bulk crystals were grown using a chemical- the sample. Namely, since a racemic crystal is not able to
vapor transport method, as described elsewhere [29]. exhibit such data, a homochiral crystalline single domain is
A micrometer-sized platelet specimen was cut from the obtained in the sample. With decreasing temperature T to
bulk single crystal used in Ref. [28] by focused ion beam 170 and 150 K, the REMC signal starts to grow. Moreover, it
methods. The sample was picked out from a particular becomes nonlinear and even oscillated as T approaches T c .
region, around which many micrometer-sized lamella The REMC behavior changes drastically below T c.
crystals were prepared for Lorentz microscopy observa- Figures 2(b)–2(d) show several notable features: a sign
tions [20] and the magnetic chirality of those samples was reversal of the REMC when below T c, sharp peaks in the
identified as left-handed. Thus, the present sample pre- vicinity of T c (at 90–120 K), a reduction of the intensity at
sumably possesses the left-handed magnetic chirality. lower T (30–70 K), and its recovery at the lowest T regime
These microscopic observations also indicate that the (below 20 K).
sample has a homochiral crystalline structure since there Figure 2(e) shows a temperature dependent REMC at
is a close correlation between the structural chirality and various magnetic fields. It is clear that the REMC signal
magnetic chirality in chiral magnetic crystals [30]. The takes negative and positive peaks above and below T c,
sample size is 13.5 × 8.5 × 0.5 μm3 . Gold electrodes for respectively. In addition, the signal becomes stronger below
four-terminal resistance measurements were fabricated in 20 K at larger fields, as seen in Fig. 2(d).

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FIG. 2. A dataset of the REMC measurements performed in a CrNb3 S6 crystal. (a)–(d) H dependence of REMC at 4.5 mA in a wider
range of temperatures. (e) T dependent REMC at 4.5 mA from 0.2 to 2.4 T with an interval of 0.2 T. (f) REMC as a function of I at 0.5 and
2 T at 110 K. The solid lines provide linear fitting curves. The inset shows the data at 200 K. (g) Angular dependence of REMC at 0.1 and
2 T at 110 K with cosine fitting curves. The insets present the data at 200 K and a geometrical relationship of H, I, θ, and c axis of the
platelet specimen.

The obtained REMC signal presents the behavior expected materials. The term S corresponds to the cross-sectional
based on Eq. (1). The signal intensity increases in pro- area of the sample.
portion to the current magnitude in the chiral conical and Negative γ̂ values are found in the PM phase as well as in
forced FM phases as well as in the PM phase, as seen in the forced FM phase and in the low T regime of the chiral
Fig. 2(f). An angular dependence of REMC in Fig. 2(g) conical phase of the present sample. In general, a magnetic
clarified that the data are well fitted by cosine curves. These contribution is largely suppressed in the PM phase with
observations guarantee the validity of Eq. (1) irrespective of increasing T, and thus the REMC observed far above T c
T. When H is applied perpendicular to I and the c axis, the should be induced mainly by the conventional EMC effect
REMC signal is almost absent, as expected for the behavior associated with chiral structures, as observed in chiral
of the CSL phase. This result also indicates that the signal is nonmagnetic materials [10,12]. The value of γ̂ is approx-
not due to the voltage derived from the Nernst effect caused imately −10−14 m2 T−1 A−1 at around 200 K in the PM
by Joule heating and justifies that the present data arise phase (a region colored in light blue), although it increases
from the EMC effect. by 1 order of magnitude with approaching T c (highlighted
Figure 3(a) presents the color contour map of the REMC in blue). Note that a typical value of the negative γ̂ obtained
intensity together with phase boundary lines. As seen in below T c is as large as −10−14 m2 T−1 A−1 , which is in the
Fig. 2, the sign of REMC changes abruptly across the phase same magnitude as the value obtained at 200 K. This result
boundary between the PM and forced FM phases. The suggests that the negative γ̂ term is originated from the
REMC signal is largely enhanced below T c, taking the crystalline chirality. It underlies in all the regions irre-
maximum value of about 300 μΩ in the chiral conical spective of T and makes a contribution in reducing the
phase. In the chiral conical phase, the amplitude of REMC REMC even in the chiral conical and forced FM phases.
reduces and its sign changes with decreasing T. A reduction Meanwhile, the positive γ̂ term becomes prominent in
in the amplitude is also seen in the forced FM phase as T three regions in which the chiral magnetic order including
decreases. However, the REMC remains positive and spin fluctuations emerges. The first region is the crossover
increases again below 20 K. regime between the PM and forced FM phases. The second
To see the REMC data in more detail, the normalized is the chiral conical phase, which exhibits large positive γ̂
EMC coefficient γ̂ is evaluated on all the magnetic phases, except for at small H and low T. The maximum value of
as shown in Fig. 3(b). Here, γ̂ is given by γ̂ ¼ γS ¼ about −10−12 m2 T−1 A−1 is obtained in the vicinity of T c .
ðS=μ0 R0 IÞ × ∂REMC =∂H, which follows Eq. (1) and is The nonreciprocal EMC transport develops significantly in
useful for analyzing the EMC effect of chiral nonmagnetic this regime. Finally, the positive γ̂ is found around the phase

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(a)

(b)

FIG. 4. (a) Magnetization curves of a CrNb3 S6 crystal in H

applied parallel to the c axis at various temperatures. (b) REMC
data with the fitting curves. The areas highlighted in light green
indicate the signal deviated from the linear behavior, which
corresponds to the nonlinear contribution ΔREMC . (c) A color
FIG. 3. Color contour maps of REMC (a) and EMC coefficient γ̂ contour map of ΔREMC on the magnetic phase diagram. Five
(b), drawn on the magnetic phase diagram of a CrNb3 S6 crystal. regions labeled by I–V are identified with the criteria of 10 μΩ.
Blue circles and black squares provide the phase boundaries (d) Temperature dependence of the EMC coefficients. Note that
determined by H and T dependent electrical resistance data, γ̂ mag takes positive values while γ̂ cryst and γ̂ max
SF take negative
respectively [31]. values in this sample.

boundary between the chiral conical phase and the forced

FM one at the low T regime. Although the magnitude of γ̂ behavior is characterized by the maximum slope in the limit
varies depending on the regions, it is natural to consider of zero magnetic field (γ̂ maxSF ). The absolute values for γ̂ mag
that the positive γ̂ term has the magnetic origin. turn out to be about 3 orders of magnitude larger than those
To distinguish crystalline and magnetic counterparts for γ̂ cryst, while the sign of them is opposite. The magnitude
explicitly, the REMC data below T c are analyzed using of γ̂ max
SF is also enhanced with regards to γ̂ cryst and its
the following empirical equation: behavior is likely to interpolate between γ̂ mag in region III
and γ̂ cryst in region V.
REMC ¼ Rcryst mag
EMC þ REMC ¼ μ0 R0 Iðγ cryst H þ γ mag MÞ: ð3Þ Possible origins of the EMC effect have been discussed
in the literature [10]. One is a self-magnetic-field effect
This equation includes the magnetic term, which varies in caused by a current-induced magnetic field on a chiral
proportion to the magnetization M of the magnetic state, as framework, which induces the REMC linearly dependent on
frequently discussed in the anomalous Hall effect [33]. H with the crystalline term γ̂ cryst . The other is a nonlinear
Figure 4(b) presents the EMC data below and above T c , chiral scattering of conduction electrons due to chiral spin
which are respectively fitted by using Eq. (3) and the fluctuations, as discussed in MnSi [34–37]. Similar critical
conventional equation without the Rmag EMC term (for details, phenomena have been found in many chiral helimagnets
see Supplemental Material [31]). A contour map of the such as FeGe [38–40], Cu2 OSeO3 [41], and CrNb3 S6
signal intensity deviated from the linear behavior, ΔREMC , [42–44]. The response of this regime is supposed to be
is provided on the magnetic phase diagram in Fig. 4(c). larger than the conventional EMC response, which is
Five regions are clearly identified. Regions II and V present consistent with the experimental results that γ̂ maxSF is larger
the linear REMC behavior. On the other hand, the signal than γ̂ cryst . These two mechanisms can explain character-
deviation ΔREMC becomes significant in regions I, III, and istics of the REMC in the PM phase. However, they do not
IV. Namely, nonlinear and field-dependent magnetic terms appear to work as the EMC mechanism which is compat-
are required for inducing the REMC behavior in those ible with the chiral magnetic order. In particular, the
regions. nonliear REMC behavior, prominent in regions I and III,
The normalized γ̂ cryst and γ̂ mag as a function of temper- is beyond the expected behavior based on Eq. (3).
ature are presented in Fig. 4(d). In region IV, the REMC Theoretical considerations on the microscopic origin of

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