Paglione Nature Phys12 2132016
Paglione Nature Phys12 2132016
Paglione Nature Phys12 2132016
Topological insulators, with metallic boundary states protected whereas it is nearly absent in the down-sweep MR data, as shown
against time-reversal-invariant perturbations1 , are a promising in Fig. 1b. Furthermore, on close inspection of the down-sweep MR
avenue for realizing exotic quantum states of matter, including data, abrupt transition-like features are apparent at low Hdn fields
various excitations of collective modes predicted in particle that are completely absent in the up-sweep data. Below 200 mK, the
physics, such as Majorana fermions2 and axions3 . According magnetoresistance abruptly drops through transition-like steps at
to theoretical predictions4 , a topological insulating state can low Hdn fields, as shown in the inset of Fig. 1b. To compare directly,
emerge from not only a weakly interacting system with strong Fig. 2a presents MR data at 100 mK obtained by systematically
spin–orbit coupling, but also in insulators driven by strong sweeping through the full ‘four-quadrant’ range, revealing a stark
electron correlations. The Kondo insulator compound SmB6 contrast between up- and down-sweep MR. This takes the form
is an ideal candidate for realizing this exotic state of matter, of a hysteretic loop that does not depend on the sign of the field,
with hybridization between itinerant conduction electrons and but only on the sweep direction. The hysteretic loop seems to close
localized f-electrons driving an insulating gap and metallic at a field of 8–10 T, with no difference in Hup or Hdn MR above
surface states at low temperatures5 . Here we exploit the that range, and vanishes if the turning field is less than 4 T (see
existence of surface ferromagnetism in SmB6 to investigate Supplementary Methods).
the topological nature of metallic surface states by studying Field-dependent hysteretic phenomena can have different ori-
magnetotransport properties at very low temperatures. We gins, but are typically associated with the presence of ferromag-
find evidence of one-dimensional surface transport with a netism. As no bulk magnetic order is observed in SmB6 according
quantized conductance value of e2 /h originating from the chiral to muon spin resonance experiments performed down to 20 mK
edge channels of ferromagnetic domain walls, providing strong (ref. 19), a surface-based FM order is the likely explanation, as
evidence that topologically non-trivial surface states exist discussed in detail below. Its hallmark signature, the anomalous
in SmB6 . Hall effect20 , is one direct way to confirm its presence. As shown
First reported over 40 years ago6 , the long-standing puzzle in Fig. 2b, the Hall resistance of SmB6 at 1 K is completely linear and
of saturating electrical resistivity in SmB6 at low tempera- negative, consistent with previous reports17,21,22 . However, at 100 mK
tures6 has recently found a possible solution7–16 . Recent transport a kink is clearly discernible in the raw data precisely near 8 T, the
experiments7,8,15,16 have proved the existence of metallic conduction field at which the hysteretic loop in MR closes. Plotted with a linear
at the surface of SmB6 crystals at temperatures much below the background subtracted, the difference 1Ryx = Ryx − AH (where A is
opening of the hybridization gap, where surface conductance dom- a linear coefficient obtained from fitting Ryx below 5 T) exhibits an
inates that of the insulating bulk of the crystal, as shown by non- abrupt onset, yet lack of hysteretic behaviour (see Supplementary
local transport7 , sample thickness dependence and surface gating Methods), as seen in Fig. 2c, suggesting that the observed Hall
studies17 . However, polarity-driven surface states14 and lack of direct resistance has an AHE term RAyx associated with FM domain align-
evidence of the chiral nature of surface conduction has brought into ment. Together with the observation of a field-history-dependent
question the topological nature of these states. In this study, we dynamics, as indicated by the presence of a strongly asymmetric
combine observations of a suppression of weak antilocalization by time relaxation in MR between Hup and Hdn (see Supplementary
spin-flip scattering, an anomalous Hall effect (AHE), a hysteretic Methods), these observations confirm without a doubt the presence
irreversibility in magnetoresistance (MR) and an unusual enhanced of FM domains.
domain wall conduction to prove the occurrence of long-range fer- Shown in Fig. 3a,b, the MR hysteresis also depends on the
romagnetic (FM) order that gaps the Dirac spectrum of the topolog- magnetic field orientation with respect to the sample. When the
ical surface states and relegates conduction to chiral edge channels. field is oriented parallel to the surface with electrical contacts
The overall magnetoresistance in SmB6 is negative at low temper- (Hk ≡ H k [010], I k [100]), the difference in up- and down-sweep
atures and varies quadratically with field, which can be attributed MR becomes vanishingly small in magnitude. As it is very unlikely
to the reduction of the Kondo energy gap by magnetic field and that a bulk-origin anomaly would break the cubic symmetry of the
the liberation of bulk charge carriers18 . The MR measurements in a crystal, it is clear that this anomalous MR hysteresis stems from a
perpendicular field orientation (H⊥ ≡ H k [001], I k [100]), obtained surface-based origin.
while applying an increasing (up-sweep) field, or Hup (Fig. 1a), are The observation of weak antilocalization (WAL) confirms this
qualitatively similar to those taken with a decreasing (down-sweep) picture. In two-dimensional conductors, weak localization appears
field, or Hdn (Fig. 1b), but with notable differences. For instance, as a quantum correction to classical magnetoresistance caused by
below 500 mK an oscillatory behaviour in the MR is visible in the constructive or destructive interference between time-reversed
the up-sweep data, reminiscent of Shubnikov–de Haas oscillations, quasiparticle paths. The presence of strong spin–orbit coupling or
Center for Nanophysics and Advanced Materials, Department of Physics, University of Maryland, College Park, Maryland 20742, USA.
*e-mail: [email protected]
a 106 b 106
Up-sweep Down-sweep
104 104
102 102
R (Ω)
R (Ω)
104
105.5
100 20 mK 100 20 mK 20 mK
100 mK 100 mK
103
R/R (300 K)
150 mK 150 mK
200 mK 105.0
100 mK 200 mK
300 mK 300 mK
102 400 mK 400 mK
500 mK 150 mK 500 mK
98 600 mK 98 104.5 600 mK
800 mK 800 mK
101
1K 200 mK 1K
0 5 10 15 20 SmB6 104.0
T (K) 0.4 0.8 1.2 1.6 2.0
96 96
0 5 10 15 0 5 10 15
μ0H (T) μ0H (T)
Figure 1 | Low-temperature magnetoresistance of topological Kondo insulator SmB6 . a, Four-wire measurements on a slab-shaped polished sample (see
Supplementary Methods) were measured in a perpendicular magnetic field orientation (H k [001], I k [100]) on increasing magnetic field, taken at constant
temperatures between 20 mK and 1 K, where surface conduction dominates that of the bulk material. The temperature dependence of resistivity in zero
field is shown in the inset, normalized to its room-temperature value. b, Magnetoresistance taken in the same perpendicular field orientation but measured
on down-sweep of field, showing qualitatively similar behaviour as for up-sweep data, but with notable differences, including a strong suppression of the
oscillatory amplitude present in up-sweep data, as well as abrupt transition-like jumps in the data as highlighted in the inset zoom (solid lines are guides to
the eye). These differences are ascribed to the presence of ferromagnetism, as described in the text.
a π Berry’s phase associated with the helical states of a topological ferromagnetism28 : in the presence of conducting Dirac electron
insulator (TI)23 changes the sign of the correction and gives rise surface states, magnetic order can be stabilized via Ruderman–
to the signature WAL enhancement of conductance, which is Kittel–Kasuya–Yosida (RKKY) interactions, and is guaranteed to be
suppressed by a time-reversal-symmetry-breaking perturbation. of the FM type if the chemical potential is close to the Dirac point
As shown in Fig. 3c,d, we observe signatures of WAL at low fields owing to a small Fermi wavenumber28 .
in both field orientations, with a strong anisotropy evident. Because We define a Curie temperature of TC ' 600 mK by the onset of
the WAL effect is normally sensitive only to the perpendicular magnetotransport hysteresis, as shown in Fig. 4a. The associated
field component, as it is an orbital effect, it is surprising to see hysteretic MR loop is, however, quite different from the conventional
any WAL correction in the Hk field orientation at all, as shown in butterfly shape commonly observed in FM materials. First, it is not
Fig. 3d. However, one must consider the finite width of the surface centred around zero magnetic field, but rather closes abruptly before
conducting state wavefunction that penetrates into the bulk with zero field is reached on down-sweep. The type of magnetization
a characteristic length λ, which combined with the rather small leading to such hysteresis is not consistent with the usual overshoot
insulating gap of SmB6 leads to a situation where orbital motion of that is necessary to overcome a coercive field, but does indeed
electrons can occur even in the Hk field orientation. occur in certain situations (see Supplementary Methods). Second,
Using the appropriate version of the Hikami–Larkin–Nagaoka the increased scattering observed in SmB6 on decreasing field (that
(HLN) equation (see Supplementary Methods), we fit the 20 mK is, R(Hdn ) > R(Hup )) is opposite to that usually observed in a ferro-
low-field sheet conductance for each field orientation, as shown in magnet, where scattering associated with domain walls is typically
Fig. 3c,d, extracting the dephasing length Lφ and the conduction enhanced on magnetization reversal. Rather, there is an enhanced
channel α parameter for each. Whereas Lφ in each field orientation conductance in SmB6 on up-sweep that is diminished on reaching
is comparable to previous results16 , the value α⊥ = 0.17 is much the closing field and returning to low fields. Interestingly, equivalent
smaller than the α = 2 × 1/2 = 1 value expected in the presence behaviour was observed in Mn-doped Bi2 (Te,Se)3 thin films tuned
of top and bottom surface conduction channels (per Dirac cone)16 . by ionic liquid gating techniques29 . In this ferromagnetic TI system,
Surprisingly, the parallel field orientation fit yields αk = 0.29, which a reversal of the usual butterfly shape occurs on gating the system
is small but still much larger than α⊥ . We attribute the overall strong into the bulk gap regime, where the TI chiral conducting modes
suppression (α < 1) and the unusual anisotropy (αk > α⊥ ) of these trapped by domain walls result in an anomalous Hall conductance
values to the presence of spin-flip scattering, which is known to associated with a quantum Hall droplet1 . In this picture, the domain
reduce the WAL effect as a result of destructive interference, leading wall conductance is enhanced during reversal of the magnetization
to α = 0 in the extreme limit where spin-flip scattering is much because the number of domain walls increases; at the coercive field,
stronger than spin–orbit scattering24,25 . where the number of the domain walls is a maximum, the conduc-
Together with MR hysteresis, the presence of spin-flip scattering tance exhibits a maximum. In SmB6 , similar behaviour is readily
suggests the existence of magnetic moments on the surface of SmB6 . shown by plotting the difference in conductance, 1G = Gup –Gdn (see
These are probably associated with samarium ions, either via the Fig. 4b), where Gup (Gdn ) is the magnetoconductance for Hup (Hdn ).
presence of unscreened f -electron Sm moments (so-called ‘Kondo With decreasing temperature, 1G is gradually enhanced and the
holes’26 ) proposed to explain logarithmic corrections to surface peak position shifts to higher field. The temperature dependence of
conductance at low temperatures16 , or possibly Sm3+ moments this characteristic field H ∗ follows a mean-field-like order parameter
in a native surface oxide layer observed by X-ray photoelectron dependence that terminates at the Curie temperature TC = 600 mK,
spectroscopy27 . With ample charge carriers present on the surface as shown in the inset of Fig. 4b. We therefore interpret H ∗ as a
of SmB6 , these moments can play a similar role to that of coercive field, in terms of the enhancement of the conductance due
magnetic impurities on the surface of a TI system in stabilizing to a maximum number of minority domains.
0.0
104
0.05
1K
ΔRyx (Ω)
105.1
Ryx (Ω)
R (Ω)
−0.2
102
100 mK
104.9 0.00
−0.4
100 H
104.7
−2 −1 0 1 2 100 mK 100 mK
−0.6 −0.05
−15 −10 −5 0 5 10 15 0 5 10 15 0 5 10 15
μ0H (T) μ0H (T) μ0H (T)
Figure 2 | Ferromagnetic hysteresis and anomalous Hall effect. a, Full ‘four-quadrant’ magnetoresistance hysteresis loop of SmB6 in perpendicular
magnetic field orientation (I k [100], H k [001]) measured at 100 mK. We observe a butterfly shape hysteresis that is sign-reversed from that of
conventional ferromagnetic materials, and is interrupted before zero field is crossed by a discontinuous jump at low field that does not depend on field sign,
as highlighted by the inset zoom. b, Anomalous Hall effect in the low-temperature Hall resistance. A prominent kink is present in low-temperature
(100 mK) data near a field of 8 T, where the hysteresis loop closes, indicating the presence of ferromagnetic order. The kink is absent at higher
temperatures (1 K), where the hysteresis in magnetoresistance also vanishes. c, Field dependence of the difference of Hall resistance 1Ryx = Ryx − AH,
where A is a linear coefficient obtained from a fitting below 5 T at 100 mK. An onset associated with the anomalous Hall effect is easily discernible at 8 T.
a 106 b
H
SmB6 SmB6
I I
50
H
104
R (Ω)
R (Ω)
49
102
100 48
100 mK 100 mK
0 5 10 15 0 5 10 15
μ 0H (T) μ 0H (T)
c 1.0 d 0.5
α = 0.17 H α = 0.29
I
Lφ = 1.2 μm I Lφ = 1.2 μm
λ = 142 nm H
0.5 0.0
ΔGs (e2/h)
ΔGs (e2/h)
0.0 −0.5
20 mK 20 mK
−0.5 −1.0
−0.10 −0.05 0.00 0.05 0.10 −0.10 −0.05 0.00 0.05 0.10
μ 0H (T) μ 0H (T)
Figure 3 | Anisotropy of low-temperature magnetoresistance hysteresis and weak antilocalization in SmB6 . a, Comparison of magnetoresistance
measured at 100 mK on sweeping magnetic field up and down (see arrows) with the field orientation perpendicular to the large surface of the sample with
contacts. A hysteretic loop is evident between a closing field of ∼10 T and a discontinuous jump at low field. b, The hysteresis is greatly suppressed when
field is oriented parallel to the measurement plane, as shown for the same sample as in a (with contacts reapplied). c, Weak antilocalization is also
observed at low fields and temperatures, but with a surprisingly small coefficient of α = 0.17 (see text) for the perpendicular field orientation. d, When the
field is applied parallel to the measurement plane, the weak antilocalization correction is much larger with α = 0.29 (see text), indicating a very strong
anisotropy opposite to that expected for the usual orbital configuration originating from the finite penetration depth λ, but consistent with strong spin-flip
scattering. Solid lines are fits to the data using the WAL correction formula (see text).
a 253 c
600 mK G1 = e2/h
251
400 mK
G (e2/h) 249 300 mK
200 mK
247
150 mK
245 100 mK
20 mK SmB6
243
0 5 10 15
μ 0H (T)
b d
H∗ CB CB
6
1.0 SS μ
μ0H∗ (T)
4
50 mK
2
20 mK
VB VB
0
Γ X/Y
ΔG (e2/h)
VB VB
0 5 10 15 Γ X/Y
μ 0H (T)
Figure 4 | Quantum conductance along surface magnetic domain wall edges. a, Magnetoconductance G of SmB6 for perpendicular field orientation
(20 mK and 100 mK data are vertically offset by −1.2e2 /h and −0.3e2 /h, respectively, for clarity). The closure of the hysteretic loop with increasing
temperature is consistent with the loss of surface ferromagnetism at a Curie temperature of ∼600 mK. The enhanced (decreased) conductance on
up(down)-sweep is opposite to that expected in conventional ferromagnetic metals, providing an indication of the topological nature of the surface
conducting states (see text). b, Magnetic field dependence of the difference of up- and down-sweep magnetoconductance 1G = Gup –Gdn . The appearance
of one quantum of conductance e2 /h in the low-temperature limit provides evidence for a scenario where surface ferromagnetism gaps the topological
conducting states within magnetic domains on the surface, limiting conductance to the domain walls. Arrows indicate the characteristic field H∗ where a
maximum in 1G is associated with a coercive field (see text). The inset presents the evolution of H∗ , consistent with the onset of ferromagnetic order at
600 mK. c, Schematic representation of the proposed grid-like ferromagnetic domain structure with walls separating domains of oppositely oriented
moments, forming a virtual random resistor network with quantized conductance components G1 = e2 /h in the presence of dissipation. The conductance
between any two non-adjacent nodes in such a network is of the order of G1 . d, Schematic band structure for SmB6 at the 0 and X/Y high-symmetry points.
Owing to the localized ordered moments, energy gaps are induced at the Dirac points, meaning the Dirac bands become massive. Because the chemical
potential µ is fixed at one value, it probably falls within the gap of one band but not in the other (see text).
Below 100 mK, the peak conductance at H ∗ reaches a value suppress ballistic quantum transport and lead to deviations from
of ∼e2 /h, a value observed in several samples with a wide range an exactly quantized conductance. The peculiar temperature- and
of residual sheet resistance values and sample dimensions (see field-dependent nature of the domain wall conductance, as well as
Supplementary Methods), indicating that the observed conductance the strong sample variation (see Supplementary Methods), provide
of e2 /h is not coincidental and possibly quantized. We suggest a picture quite consistent with this situation.
that the quantized conductance signature originates from transport Furthermore, the presence of a grid-like FM domain struc-
of massive Dirac carriers along one-dimensional channels that ture introduces another degree of complexity in the presence of
lie between FM domains. In this scenario, the domain wall dissipation. Provided the characteristic FM domain size is suffi-
conductance is equal to the anomalous quantum Hall conductance, ciently smaller than the approximately mm-scale sample dimension,
quantized as (n + 1/2)e2 /h, as expected in a massive Dirac the domain walls will effectively form an infinite resistor (con-
spectrum induced by FM ordered moments pointing out of the ductor) network with R1 = h/e2 (G1 = e2 /h) elements, as shown
surface plane1,30 . in Fig. 4c. The dissipation or puddling is equivalent to virtual
In an ideal system with no dissipation, ballistic transport should removal of resistors at random from the network, yielding the
occur and exactly quantized conductance should be observed, formation of a random network which consists of a conductance
as is the case for refs 31,32. However, in non-ideal systems G1 = e2 /h distributed randomly with a probability of p and a con-
the chiral surface states suffer from abundant inelastic scattering ductance G2 = 0 distributed randomly with a probability of 1 − p.
due to electron correlations33 or the ‘puddling’ effect of spatial In such a random network, the percolating conduction gives the
variations in the electronic structure34 , both of which easily equivalent conductance between any two non-adjacent nodes of