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High-temperature quantum inset, and fig. S1) made from graphene super-
lattices (26) to carry out our transport measure-
ments. Monolayer graphene was placed on top
oscillations caused by recurring of a hexagonal boron nitride (hBN) crystal, and
their crystallographic axes were aligned with an
Bloch states in graphene superlattices accuracy of better than 2° (17, 24). The resulting
moiré pattern gives rise to a periodic potential
that is known to affect the electronic spectrum
R. Krishna Kumar,1,2,3 X. Chen,2 G. H. Auton,2 A. Mishchenko,1 D. A. Bandurin,1 of graphene (23–25). To ensure that the charge
S. V. Morozov,4,5 Y. Cao,2 E. Khestanova,1 M. Ben Shalom,1 A. V. Kretinin,2,6 carriers have high mobility, the graphene was
K. S. Novoselov,2 L. Eaves,2,7 I. V. Grigorieva,1 L. A. Ponomarenko,3 encapsulated using a second hBN crystal, which
V. I. Fal’ko,1,2* A. K. Geim1,2* was intentionally misaligned by ~15° with respect
to graphene’s axes. Although the second hBN
Cyclotron motion of charge carriers in metals and semiconductors leads to Landau layer also leads to a moiré pattern, it has a short
quantization and magneto-oscillatory behavior in their properties. Cryogenic periodicity and, accordingly, any superlattice ef-
temperatures are usually required to observe these oscillations. We show that graphene fects may appear only at high carrier concentra-
O
cedures but with the graphene misaligned with
scillations of physical properties of mate- normally requires low temperatures (T), and this respect to both top and bottom hBN layers.
rials with magnetic field are a well known requirement is particularly severe in the case of Figure 1A shows typical behavior of the longi-
and important phenomenon in condensed quantum oscillations that rely on the monochro- tudinal resistivity rxx for graphene superlattices
matter physics. Despite having a variety of maticity of interfering electron waves. Even in as a function of B at various T. For comparison,
experimental manifestations, there are only graphene, with its massless Dirac spectrum and Fig. 1B plots similar measurements for the ref-
a few basic types of oscillations: those of either exceptionally large cyclotron gaps, SdH oscilla- erence device. In the latter case, rxx exhibits pro-
quantum or semiclassical origin (1–5). Semiclas- tions rarely survive above 100 K. At room T, high nounced SdH oscillations at liquid-helium T, which
sical size effects, such as Gantmakher and Weiss magnetic fields (B) of ~30 T are needed to observe develop into the quantum Hall effect above a few
oscillations, appear owing to commensurability the last two SdH oscillations arising from the maxi- tesla. The SdH oscillations are rapidly suppres-
between the cyclotron orbit and a certain length mal gaps between the zeroth and first Landau sed with increasing T and completely vanish above
in an experimental system (1–4). Quantum magneto- levels (LLs) of graphene (6). In all other ma- liquid-nitrogen T, the standard behavior for
oscillations are different in that they arise from terials, quantum oscillations disappear at much graphene in these relatively weak fields (27, 28).
periodic changes in the interference along closed lower T. In stark contrast, graphene superlattices exhibit
electron trajectories (1–5). Most commonly, quan- Electronic systems with superlattices can also prominent oscillations over the entire T range
tum oscillations involve cyclotron trajectories. This exhibit magneto-oscillations. In this case, the inter- (Fig. 1A and fig. S2). At both high and low T, the
leads to Landau quantization and, consequently, ference of electrons diffracting at a superlattice oscillations are periodic in 1/B (figs. S3 and S4).
Shubnikov–de Haas (SdH) oscillations in mag- potential in a magnetic field results in fractal, The oscillations in Fig. 1A change their frequency
netoresistance and the associated oscillatory be- self-similar spectra that are often referred to as at ~50 K. This is the same T range in which SdH
havior in many other properties (1–3). In addition, Hofstadter butterflies (HBs) (7–12). Their fractal oscillations disappear in the reference device of
quantum oscillations may arise from interference structure reflects the fact that charge carriers ef- Fig. 1B. For certain ranges of n and B, we observed
on trajectories imposed by sample geometry, lead- fectively experience no magnetic field if mag- that SdH oscillations vanished first, before new
ing to Aharonov-Bohm oscillations in mesoscopic netic flux f through the superlattice unit cell is oscillations emerged at higher T. An example of
rings, for instance (3, 5). Whatever their exact commensurate with the magnetic flux quantum, such nonmonotonic T dependence is shown in
origin, the observation of such oscillatory effects f 0 (7–9). This topic has attracted interest for fig. S2. To emphasize the robustness of the high-
decades (11–16) but received a particular boost T oscillations, we show that they remain well
1
School of Physics and Astronomy, University of Manchester,
thanks to the recent observation of clear self- developed even at boiling-water T in moderate
Manchester M13 9PL, UK. 2National Graphene Institute, similar features in transport characteristics and B (Fig. 1C). The oscillations were observed even
University of Manchester, Manchester M13 9PL, UK. in the density of states (DOS) of graphene superlat- at higher T, but above 400 K our devices (both
3
Department of Physics, University of Lancaster, Lancaster tices (17–25). Because the HB depicts quantum states superlattice and reference devices) showed rapid
LA1 4YW, UK. 4Institute of Microelectronics Technology and
High Purity Materials, Russian Academy of Sciences,
developed from partial admixing of graphene’s deterioration in quality and strong hysteresis as
Chernogolovka 142432, Russia. 5National University of original LLs (12), superlattice-related gaps already a function of gate voltage.
Science and Technology (MISiS), Moscow 119049, Russia. become smeared at relatively low T, well below The high-T and SdH oscillations differ not only
6
School of Materials, University of Manchester, Manchester those at which signatures of quantization in the in their periodicity and thermal stability but also
M13 9PL, UK. 7School of Physics and Astronomy, University
of Nottingham, Nottingham NG7 2RD, UK.
main spectrum disappear. Therefore, it is perhaps because they have distinctly different n depen-
*Corresponding author. Email: vladimir.falko@manchester.ac.uk not surprising that investigations of Hofstadter dences. Figure 2, A and B, shows Landau fan dia-
(V.I.F.); geim@manchester.ac.uk (A.K.G.) systems were confined mostly to low T. As shown grams for the longitudinal conductivity sxx of
Δρxx (Ω)
ρxx (Ω)
ρxx (Ω)
600
ρxx (Ω)
150 K 150 K Reference graphene
300
25
100 K
100 K 400
30
50 K
50 K
150 0
200
10K 10 K
Fig. 1. High-temperature oscillations in graphene superlattices. by a factor of 4. Dotted curves: Oscillatory behavior is emphasized by
(A) rxx at relatively small B for a superlattice device with a moiré periodicity subtracting a smooth background, using fourth-order polynomials as best
of ≈13.6 nm. The electron density is n ≈ 1.7 × 1012 cm−2 and is induced by fits to the original rxx curves (26). At 100°C, graphene superlattices
a back-gate voltage. (Inset) Optical micrograph of one of our Hall bar exhibit oscillations starting below 4 T, whereas no sign of oscillatory
devices. Scale bar, 5 mm. W, ohms. (B) Same as (A) but using the reference behavior could be discerned at this T in our reference devices at any
10 10 10
φ0/φ = 3
8 8 8
4
6 6 6 35 B0 (T)
B (T)
B (T)
B (T)
5
6 30
4 4 7 4
25
2 2 2
2.4 2.8 3.2
10 K 150 K
n0 (1012 cm-2) 150 K
0 0 0
-1 0 1 -1 0 1 -1 0 1
n/n0 n/n0 n/n0
-5
10 7
9
Δσxx, e2/h 7
Δσxy, e2/h
6 -3
1.5
3
0.1
0
8 zero Beff 6 -3 6 3
σxx
σxx, σxy (mS)
-6 5
σxy 1.0
φ0/φ
φ0/φ
6
5 5
4
0.5 4 4
2
zero Beff 150 K
n/n0 = 1.5 3 3
0 0
0 3 6 9 12 0.8 1.2 1.6 0.8 1.2 1.6
B (T) n/n0 n/n0
Fig. 2. Concentration and field dependence of Brown-Zak (BZ) oscil- (dashed lines are for q = 3 to 6), local changes in sxx and sxy resemble
lations. (A) Low-T fan diagram sxx(n, B) for a superlattice device with a ≈ magnetotransport in metals near zero field, as illustrated by the green inset
13.9 nm. The gray scale is logarithmic: white, 0.015 mS; black, 15 mS. curves. (E) Part of (C) near the second-generation NP for electron doping
(B) Same device as (A) but at 150 K. Logarithmic gray scale: white, 0.1 mS; is magnified and plotted as a function of f 0 =f. The main maxima in Dsxx
black, 10 mS. The dotted lines denote B ¼ f 0 =qS. (C) Same as (B) but for occur at f 0 =f ¼ q. A few extra maxima for p = 2 and 3 are indicated by black
Dsxx obtained by subtracting a smooth best-fit background (26). Linear gray and green arrows, respectively (see fig. S6 for details). (F) Corresponding
scale: ±0.3 mS. (Inset) Fundamental frequency B0 of BZ oscillations found in behavior of Dsxy (smooth background subtracted). Its zeros align with the
pffiffiffi
our different devices as a function of n0 ¼ 8= 3a2 . (D) Near B ¼ f 0 =qS red maxima in Dsxx.
( m S)
(top and bottom panels, Brown (7) and Zak (8) and predates the work by
respectively) in a super- Hofstadter (10). Examples of BZ minibands for
lattice device with a ≈
ε ky several unit fractions of f 0 are shown in Fig. 3
xx
13.6 nm. Black dots and 10
σ and fig. S8, using a generic graphene-on-hBN
curves: sxx calculated in kx potential (26). Each miniband can be viewed as a
the constant-t approxi- superlattice-broadened LL, such that its energy
→
mation for different p and 5 dispersion eðk Þ disappears in the limit of vanish-
q. Inset image: BZ mini- ing superlattice modulation (12). If the Fermi
→
bands eðk Þ inside the first energy eF lies within these superlattice-broadened
Brillouin zones indicated LLs, the system should exhibit a metallic behavior
( m S)
by the gray hexagons Valence band (25). The Hofstadter spectrum can then be under-
(their size decreases with stood as Landau quantization of BZ minibands
increasing q). The mini- 1
in the effective field Beff ¼ B f 0 p=qS (20, 29).
xx
bands were calculated for With this concept in mind, let us take a closer
σ
a generic graphene-on-
0 look at the experimental behavior of sxx and
hBN superlattice (29) 0 the Hall conductivity sxy at high T and small
coefficient. It can be evaluated (26) without chromaticity, which allows them to persist up to 14. C. Albrecht et al., Phys. Rev. Lett. 86, 147–150 (2001).
extra fitting parameters (narrow black parab- exceptionally high T, beyond the existence of 15. M. C. Geisler et al., Physica E 25, 227–232 (2004).
16. S. Melinte et al., Phys. Rev. Lett. 92, 036802 (2004).
olas in Fig. 3). One can see that the theory pro- LLs. The extrapolation of the observed T depen- 17. L. A. Ponomarenko et al., Nature 497, 594–597 (2013).
vides qualitative agreement for the observed dences (fig. S4B) suggests that the quantum oscil- 18. C. R. Dean et al., Nature 497, 598–602 (2013).
experimental peaks. The derived values of t yield lations may be observable even at 1000 K. Further 19. B. Hunt et al., Science 340, 1427–1430 (2013).
sxx(B = 0) ≈ 20 mS, again in qualitative agree- theory is required to understand details of tem- 20. G. L. Yu et al., Nat. Phys. 10, 525–529 (2014).
ment with experiment. It would be unreasonable perature, field, and concentration dependences 21. L. Wang et al., Science 350, 1231–1234 (2015).
22. W. Yang et al., Nano Lett. 16, 2387–2392 (2016).
to expect any better agreement because of the of BZ oscillations; the origin of the electron-hole
23. M. Yankowitz et al., Nat. Phys. 8, 382–386 (2012).
limited knowledge about the graphene-on-hBN asymmetry of phonon scattering; the behavior 24. C. R. Woods et al., Nat. Phys. 10, 451–456 (2014).
superlattice potential (20, 29) and the used t of higher-order fractions; and the effect of inter- 25. Z. G. Chen et al., Nat. Commun. 5, 4461 (2014).
approximation. The observed exponential T de- miniband scattering, which is responsible for the 26. See supplementary materials.
pendence of BZ oscillations (detailed in fig. S4) non-oscillating background. 27. K. S. Novoselov et al., Nature 438, 197–200 (2005).
can also be understood qualitatively as arising 28. Y. Zhang, Y. W. Tan, H. L. Stormer, P. Kim, Nature 438,
201–204 (2005).
from scattering on acoustic phonons such that the 29. X. Chen et al., Phys. Rev. B 89, 075401 (2014).
RE FERENCES AND NOTES
scattering length ðº1=T Þ becomes shorter than 30. N. M. Freitag et al., Nano Lett. 16, 5798–5805 (2016).
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AC KNOWLED GME NTS
To conclude, graphene superlattices exhibit a Press, 1980). This work was supported by the European Research Council,
3. C. W. J. Beenakker, H. van Houten, Solid State Phys. 44, 1–228 Lloyd’s Register Foundation, the Graphene Flagship, and the
distinct quantum oscillatory phenomenon that Royal Society. R.K.K. and E.K. acknowledge support from the
(1991).
can be understood as repetitive formation of dif- 4. R. R. Gerhardts, D. Weiss, Kv. Klitzing, Phys. Rev. Lett. 62, Engineering and Physical Sciences Research Council, D.A.B. and
ferent metallic systems, the BZ minibands. At 1173–1176 (1989). I.V.G. from the Marie Curie program SPINOGRAPH, and S.V.M.
simple fractions of f 0 , charge carriers effectively 5. R. A. Webb, S. Washburn, C. P. Umbach, R. B. Laibowitz, Phys. from the Russian Science Foundation and National University of
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