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PHYSICAL REVIEW LETTERS 130, 136301 (2023)

Editors' Suggestion

Giant Magnetochiral Anisotropy in Weyl Semimetal WTe2 Induced


by Diverging Berry Curvature
Tomoyuki Yokouchi ,1,* Yuya Ikeda ,2 Takahiro Morimoto ,2 and Yuki Shiomi1
1
Department of Basic Science, The University of Tokyo, Tokyo 152-8902, Japan
2
Department of Applied Physics, The University of Tokyo, Tokyo 113-8656, Japan
(Received 18 November 2022; accepted 8 March 2023; published 30 March 2023)

The concept of Berry curvature is essential for various transport phenomena. However, an effect of the
Berry curvature on magnetochiral anisotropy, i.e., nonreciprocal magnetotransport, is still elusive. Here, we
report that the Berry curvature induces the large magnetochiral anisotropy. In Weyl semimetal WTe2 , we
observe the strong enhancement of the magnetochiral anisotropy when the Fermi level is located near the
Weyl points. Notably, the maximal figure of merit γ̄ reaches 1.2 × 10−6 m2 T−1 A−1 , which is the largest
ever reported in bulk materials. Our semiclassical calculation shows that the diverging Berry curvature at
the Weyl points strongly enhances the magnetochiral anisotropy.

DOI: 10.1103/PhysRevLett.130.136301

Whether physical responses are allowed or prohibited is The magnetochiral anisotropy effect (also called the nonre-
closely related to symmetries [1]. For example, in the linear ciprocal magnetotransport effect) is nonreciprocal transport
response regime, the anomalous Hall effect is allowed when responses triggered by an external magnetic field; under
time-reversal symmetry is broken [2]. In contrast, the spin magnetic fields, the longitudinal and transverse resistivity of
Hall effect is allowed independent of both time-reversal and a material is different for electric current I flowing to
crystalline symmetries [2]. In the nonlinear response the right (þI) and to the left (−I). The magnetochiral
regime, a nonlinear Hall effect without external magnetic anisotropy effect essentially differs from the nonlinear
field is allowed in a bilayer WTe2 but prohibited in a bulk Hall effect, since the former requires time-reversal symmetry
WTe2 due to the difference in the crystalline symmetries breaking but the latter does not. Hence, physical mechanisms
between them [3,4]. In addition, the bulk photovoltaic different from the nonlinear Hall effect must exist in the
effect, a nonlinear optical phenomenon, is allowed in a magnetochiral anisotropy effect. So far, several underlying
system without spatial inversion symmetry [4–6]. Beyond mechanisms of the magnetochiral anisotropy effect have
the symmetry argument, the microscopic mechanisms of been clarified. For example, an asymmetric electron scatter-
these physical phenomena have been intensively studied. ing [17,18,21,22,30] and the magnetic-field-induced defor-
An important finding is that the notion of the Berry mation of the Fermi surface caused by the Zeeman term
curvature of an electronic wave function is essential for [16,19] have been identified as the microscopic mechanisms.
the description of these phenomena [7]. For example, the From the viewpoint of symmetry, modification of electron
intrinsic anomalous and spin Hall effects are proportional to motion due to the Berry curvature is also expected to affect
the integral of Berry curvature over the Fermi sea [2]. In the magnetochiral anisotropy effect since the momentum-
addition, recently, it was found that the Berry curvature also integrated Berry curvature can be nonzero in systems with
manifests itself in nonlinear responses; the nonlinear Hall broken time-reversal symmetry. However, the role of the
effect under time-reversal symmetry is induced by the Berry curvature on the magnetochiral anisotropy effect has
dipole moment of the Berry curvature [3,4,8,9]. In one of not been well explored.
the microscopic mechanisms of the bulk photovoltaic effect To study the effect of Berry curvature on the magneto-
(shift current mechanism), the photocurrent is quantified by chiral anisotropy effect, Weyl semimetals with broken
the difference in the Berry connection between the valance spatial inversion symmetry [31,32] are a suitable candidate.
and conduction bands [10,11]. Hence, investigating the Weyl semimetals are quantum materials characterized by
relationship between the Berry curvature and a physical topologically nontrivial band structure and possess pairs of
response has been one of the central issues in modern band crossing points termed Weyl points. The Weyl points
condensed matter physics. act as monopoles of the Berry curvature, and the Berry
Only when the time-reversal and spatial inversion curvature becomes singular and diverges at the Weyl points.
symmetries are simultaneously broken another class of Hence, when the Fermi level is located near the Weyl
the nonlinear responses is allowed, that is, the magneto- points, the effect of the Berry curvature is maximized, and
chiral anisotropy effect [12–30] which we focus on here. thus, the magnetochiral anisotropy effect is expected to be

0031-9007=23=130(13)=136301(6) 136301-1 © 2023 American Physical Society


PHYSICAL REVIEW LETTERS 130, 136301 (2023)

dramatically enhanced. In this Letter, we demonstrate this effect have not been well investigated when the Femi
scenario using bulk crystals of a polar Weyl semimetal level is tuned near the Weyl points hosting diverging
WTe2 . The symmetry of bulk WTe2 is a Pmn21 (polar), Berry curvature.
and WTe2 possesses four pairs of Weyl points [33–35]. In Figs. 1(d) and 1(e), we present the magnetic-field
Around the Weyl points, the Berry curvature is strongly dependence of the second-harmonic Hall effect and the
enhanced as schematically shown in Fig. 1(a). nonreciprocal magnetoresistance in bulk WTe2 whose
Generally, the direction of the electric field generated in Fermi level is close to the Weyl points (sample F).
the magnetochiral anisotropy effect depends on the mag- Here, we evaluate the Fermi-level position from the carrier
netic-field direction [12]. The presence of the mirror plane densities of electrons and holes obtained by the Hall
in WTe2 constrains the expected direction of the voltage resistivity measurement (see Ref. [36] for details). Because
drop induced by the magnetochiral anisotropy responses in the magnetochiral anisotropy effect is proportional to the
WTe2 as shown in Figs. 1(b) and 1(c); the longitudinal magnitude of the square of the current density j2, we
response (hereafter called nonreciprocal magnetoresist- measured the second-harmonic longitudinal and transverse
ance) is proportional to sin θ and largest when the magnetic resistivity (ρ2f 2f
xx and ρyx ) (see also Ref. [36] for details). In
field (H) is perpendicular to the current. Here, θ is the accord with the expected contribution from the magneto-
relative angle between the magnetic-field direction and the chiral anisotropy effect, the field profiles of ρ2f 2f
xx and ρyx are
current direction. In contrast, the transverse response
antisymmetric against the magnetic field. Here, ρxx and ρ2f2f
yx
(hereafter called second-harmonic Hall effect) is propor-
are antisymmetrized with respect to the magnetic field (see
tional to cos θ and largest when H is parallel to the current.
also Ref. [36]). The field profiles of the nonreciprocal
Here, we note although the nonreciprocal magnetoresist-
magnetoresistance and the second-harmonic Hall effect
ance was reported in nanometer-thick WTe2 whose Fermi
level is apart from the Weyl points [19], both the nonre- before antisymmetrization [ρ2f 2f
xx;meas ðHÞ and ρyx;meas ðHÞ] is

ciprocal magnetoresistance and the second-harmonic Hall also antisymmetric against the magnetic field as shown in
the Supplemental Material Fig. S5 [36]. The magnitude of
the magnetochiral anisotropy can be represented by γ̄ xx
(a) E ky and γ̄ yx , which are independent of the sample size and
defined by EMCA x ¼ ρxx γ̄ xx Bj2 and EMCA y ¼ ρxx γ̄ yx Bj2 ,
respectively. Here, E MCA is the magnetochiral anisotropy
kx
x
electric field, and γ̄ xx and γ̄ yx are related to ρ2f 2f
xx and ρyx as
γ̄ xx ¼ −2ρ2f 2f
xx =ðρxx jBÞ and γ̄ yx ¼ −2ρyx =ðρxx jBÞ [36]. The
obtained magnitudes of jγ̄ yx j and jγ̄ xx j are as large as
1.2 × 10−6 and 0.34 × 10−6 m2 T−1 A−1 at 1 T, respectively.
Remarkably, γ̄ yx is much larger than the previously reported
(b) second-harmonic Hall effect (c) nonreciprocal magnetoresistance
γ̄ yx values in bulk materials [41], and γ̄ xx is almost identical
Vyx2f to the previously reported largest value of γ̄ xx in ZrTe5 [28].
I Vxx2f
Interestingly, the second-harmonic Hall effect (i.e., ρ2f yx for
H
H==I) is larger than the nonreciprocal magnetoresistance
(d) (e)
(i.e., ρ2f
0.4 0.4
xx for H ⊥I) [Figs. 1(d) and 1(e)]. This feature cannot
0.2 0.2 be explained by the previously reported asymmetric elec-
/ρxx

/ρxx

0.0 0.0 tron scattering mechanism, in which the magnitude of the


yx

xx

second-harmonic Hall effect and the nonreciprocal mag-


2f

2f
ρ

-0.2 -0.2
netoresistance must be the same [18]. As will be discussed
-0.4 -0.4 later, this difference originates from the effects of the Berry
-8 -6 -4 -2 0 2 4 6 8 -8 -6 -4 -2 0 2 4 6 8
μ0H (T) μ0H (T) curvature and the chiral anomaly.
To further confirm that the observed signals originate
FIG. 1. (a) Schematics of the energy dispersion for a type-II from the magnetochiral anisotropy effect, first, we inves-
Weyl semimetal near a Weyl point and the Berry curvature (Ωx ) tigated the dependence of ρ2f yx with H==I on the input-
around the Weyl points in WTe2 . The black and gray circles current frequency (f) and on the current density (j) in
represent Weyl points with the chirality η ¼ þ1 and −1, sample A. The Fermi level of sample A is also located near
respectively. Experimental configurations for (b) the second-
the Weyl points as in sample F. As expected in the second-
harmonic Hall effect and (c) the nonreciprocal magnetoresist-
ance. Magnetic-field dependence of (d) the second-harmonic Hall harmonic Hall effect, the magnitude of ρ2f yx is independent
effect and (e) the nonreciprocal magnetoresistance in sample F of f and linearly increases with increasing j in the low
measured with j ¼ 8.8 × 105 Am−2 and f ¼ 33 Hz at 5 K. The current density region [Figs. 2(a) and 2(c)]. Note that the
current direction is parallel to the b axis. deviation from the linear relationship in Fig. 2(c) at high

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PHYSICAL REVIEW LETTERS 130, 136301 (2023)
sample A, I // a axis,
(a) (b)
H I H I H I
(a) 0.01
(c)
Vyx2f
0.00
θ

ρyx / ρxx
-0.01

2f
-0.02
(d) 1 T, 5 K
-0.03
-90 -60 -30 0 30 60 90
θ (deg.)
(b) 13
(e) (g) 10 sample A 1T

|σxxx| (A/V T)
11
10

2
9
10
(f) (h) sample F
7
10
5
10
(c) 13
10
1T
FIG. 2. (a) Frequency dependence of ρ2f yx and (b) current |σxyy| (A/V T) 11
10 sample F
2

density dependence of the estimated temperature of the sample


and (c) of ρ2f yx in sample A. The frequency dependence is 9
10
measured with j ¼ 0.44 × 106 Am−2 , and the current depend-
ence is measured with f ¼ 53 Hz. The current direction is 10
7

parallel to the a axis. (d) Schematic of the fabrication of samples sample A


5
D and L, in which the polarity directions are opposite each other. 10
(e)–(h) Magnetic-field dependence of the second-harmonic 0 20 40 60 80 100
Hall effect in sample D and sample L and the nonreciprocal T (K)
magnetoresistance in sample D and sample L measured with
j ¼ 1.2 × 106 Am−2 and f ¼ 33 Hz. FIG. 3. (a) Angular dependence of ρ2f yx =ρxx measured with
j ¼ 8.8 × 105 Am−2 , f ¼ 3.3 Hz, and I==a axis. The definition
of θ is shown in the inset. The blue lines are fits to cos θ. (b),(c)
current is attributed to the temperature increase due to the Temperature dependence of jσ xyy j ¼ 2jρ2f 3
yx jj=ρxx B and jσ xxx j ¼
2f
Joule heating effect; the maximum temperature increase is 2jρxx jj=ρ3xx B at 1 T in samples A and F. The current density for
approximately 5 K [Fig. 2(b)], which is estimated from the sample A and sample F is j ¼ 8.8 × 105 and 3.4 × 105 Am−2 ,
change in the linear longitudinal resistivity. Then, we respectively. The current direction is parallel to the a axis in
investigated polarity-direction dependence; the sign of the sample A and the b axis in sample F. The frequency of the current
second-harmonic Hall effect and the nonreciprocal is f ¼ 33 Hz in both samples.
magnetoresistance should be reversed when the polarity
direction is reversed [12]. We divided a WTe2 sample into addition, as a cross-check, we reproduced the magnetochiral
two (samples D and L) so that the polarity directions are anisotropy in dc measurements [36].
opposite each other [Fig. 2(d)]. As shown in Figs. 2(e)–2(h), Then, we investigate the temperature dependence of the
the signs of ρ2f 2f
yx =ρxx and ρxx =ρxx are opposite for samples D second-harmonic Hall effect and the nonreciprocal mag-
and L, in accord with the expected trends in the second- netoresistance. In Figs. 3(b) and 3(c), we show the temper-
harmonic Hall effect and the nonreciprocal magnetoresist- ature dependence of jσ xyy j and jσ xxx j at 1 T for sample A and
ance. We also measured ρ2f yx =ρxx as a function of the relative
sample F. Here, σ xyy and σ xxx are defined as jx ¼ σ xyy E2y B
angle (θ) between the magnetic-field direction and the and jx ¼ σ xxx E2x B and related to ρ2f 2f
yx and ρxx as σ xxx ¼
2f 2f
current direction. As shown in Fig. 3(a), ρ2f yx =ρxx obeys
3 3
−2ρxx j=Bρxx and σ xxx ¼ 2ρyx j=Bρxx , respectively [36].
cos θ as expected. These results corroborate that the observed As can be seen from Figs. 3(b) and 3(c), the absolute
signals originate from the magnetochiral anisotropy effect. In values of σ xyy and σ xxx increase notably with decreasing

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PHYSICAL REVIEW LETTERS 130, 136301 (2023)

temperature. The enhancement at low temperatures should the ratio of the change in the calculated nonreciprocal
be closely related to the microscopic mechanism and will be response is less than 10 as a function of the Fermi-level
discussed later. position.
Next, we investigated the Fermi-level dependence of the The observed Fermi-level dependence of the magneto-
second-harmonic Hall effect and the nonreciprocal man- chiral anisotropy effect can be understood by a semiclassical
getoresistance. In WTe2 , it is known that the Fermi-level treatment of current responses including the contribution
position changes due to a deficiency of Te and can be from the Berry curvature. We use the Boltzmann equation to
evaluated by the ratio between the hole carrier density (nh ) derive momentum distribution under the electric field and
and the electron carrier density (ne ) [42]. According to the the magnetic field and calculate the second-harmonic Hall
previous study [42], when the Fermi level is close to the and nonreciprocal magnetoresistance responses (for details,
Weyl points, ne =nh is approximately 1.08. Hence, we see Ref. [36]). We find that the combination of C2 rotation
measured γ̄ yx and γ̄ xx in more than ten samples and plot symmetry of WTe2 around the z direction and the time-
the absolute value of γ̄ yx and γ̄ xx at 1 T as a function of reversal symmetry leads to a constraint that the transverse
ne =nh (see also Refs. [36,43] for the evaluation of ne and nonlinear conductivity σ xyy and longitudinal nonlinear
nh ). As shown in Figs. 4(a) and 4(b), jγ̄ yx j and jγ̄ xx j conductivity σ xxx are proportional to the square of the
systematically depend on ne =nh , or equivalently, the relaxation time τ. The semiclassical treatment shows that
Fermi-level position. Notably, both jγ̄ yx j and jγ̄ xx j change such τ2 contribution to the second-harmonic Hall current
by more than 4 orders of magnitude and are largest when arises from energy shift due to the orbital magnetic moment
the Fermi level is close to the Weyl points. We note that this and the momentum shift related to chiral anomaly. These
Fermi-level dependence of jγ̄ yx j ¼ jρ2f yx j=ρxx and jγ̄ xx j ¼
effects are substantially enhanced when the Fermi energy
is close to the Weyl point reflecting the diverging Berry
jρxx j=ρxx mainly results from that of ρyx and ρ2f
2f 2f
xx ; as shown
curvature around the Weyl point. Therefore, as shown in
in Fig. S9 of the Supplemental Material [36], ρxx is almost
Figs. 4(c) and 4(d), large second-harmonic Hall and
independent of the Fermi-level position. The observed
nonreciprocal magnetoresistance responses appear when
substantial increase in the magnetochiral anisotropy
the Fermi energy is tuned close to the Weyl points, which
responses around the Weyl points cannot be explained
is qualitatively consistent with the observed enhancement
by the previously reported semiclassical calculation of the
of the second-harmonic Hall effect and the nonreciprocal
nonreciprocal responses in WTe2 [19], in which an effect of
magnetoresistance. In particular, when the Fermi energy is
the Berry curvature is not included; in this previous work,
located between the Weyl and anti-Weyl points, the con-
tribution from the two nodes adds up in a constructive way,
leading to giant magnetochiral anisotropy.
(a) (c)
Our theory can also explain the experimentally observed
difference in the magnitudes of the second-harmonic Hall
effect and the nonreciprocal magnetoresistance. As already
shown in Figs. 1(d) and 1(e), the magnitude of the second-
harmonic Hall effect is larger than that of the nonreciprocal
magnetoresistance in sample F. Furthermore, all other
(b) (d)
samples also have the same relationship regardless of the
current direction with respect to the crystalline axis; as
presented in Figs. 4(a) and 4(b), the magnitude of the second-
harmonic Hall effect is larger than that of the nonreciprocal
magnetoresistance for each sample. In the theory, as can be
seen from Eq. S11 in the Supplemental Material [36], the
second order current contains the E · B term that originates
from the chiral anomaly [44,45]. Since the E · B term is
FIG. 4. (a),(b) Absolute values of γ̄ yx ¼ −2ρ2f yx =ρxx jB and largest for j==B (the second-harmonic Hall configuration)
γ̄ xx ¼ −2ρ2f
xx =ρ xx jB as a function of the ratio between electron and zero for j⊥B (the nonreciprocal magnetoresistance
carrier density (ne ) and hole carrier density (nh ). The circle and configuration), the second-harmonic Hall effect is always
triangle points are samples measured with I==b axis and I==a larger than the nonreciprocal magnetoresistance if the Fermi-
axis, respectively. The upper panel schematically denotes the
level position is the same. Furthermore, the present theory is
position of the Fermi level corresponding to the value of ne =nh .
The region where the Fermi level is close to the Weyl points is also consistent with the experimentally observed temperature
denoted by the red shadow. (c),(d) Absolute values of γ̄ yx and γ̄ xx dependence of σ xyy and σ xxx ; both σ xyy and σ xxx increase with
as a function of the Fermi energy obtained from the semiclassical decreasing temperature [see Figs. 3(b) and 3(c)]. Since σ xyy
calculation. We set the magnetic field B ¼ 10−5 ℏ=ea2 and the and σ xxx in our theory are proportional to the square of
energy separation of the two Weyl points ΔE ¼ 0.04 vF ℏ=a. the relaxation time, they should increase with decreasing

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PHYSICAL REVIEW LETTERS 130, 136301 (2023)

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This work was supported by JST FOREST Program [17] T. Yokouchi, N. Kanazawa, A. Kikkawa, D. Morikawa, K.
(Grant No. JPMJFR203H), JST PRESTO (Grant No. Shibata, T. Arima, Y. Taguchi, F. Kagawa, and Y. Tokura,
Electrical magnetochiral effect induced by chiral spin
JPMJPR19L9), JST CREST (Grant No. JPMJCR19T3),
fluctuations, Nat. Commun. 8, 866 (2017).
JSPS KAKENHI (Grants No. 22H04464, No. 22H05449, [18] K. Yasuda, A. Tsukazaki, R. Yoshimi, K. Kondou, K. S.
No. 21K18890, No. 21H01794, No. 19H05600, and Takahashi, Y. Otani, M. Kawasaki, and Y. Tokura, Current-
No. 19K14667), and the Murata Science Foundation. Nonlinear Hall Effect and Spin-Orbit Torque Magnetization
Switching in a Magnetic Topological Insulator, Phys. Rev.
Lett. 119, 137204 (2017).
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